Updated on 2024/03/16

写真a

 
TAKAHASHI Yasufumi
 
Organization
Graduate School of Engineering Electronics 2 Professor
Graduate School
Graduate School of Engineering
Undergraduate School
School of Engineering Electrical Engineering, Electronics, and Information Engineering
Title
Professor

Degree 1

  1. 博士(学術) ( 2009.3 ) 

Research Areas 1

  1. Nanotechnology/Materials / Analytical chemistry  / 走査型プローブ顕微鏡

Research History 8

  1. Nagoya University   Graduate School of Engineering Electronics   Professor

    2021.12

  2. Kanazawa University   Professor

    2020.10

  3. Kanazawa University   Associate professor

    2017.10 - 2020.9

  4. Kanazawa University   Associate professor

    2015.10 - 2017.9

  5. Tohoku University   Assistant Professor

    2013.4 - 2015.9

  6. Tohoku University Advanced Institute for Materials Research, Device/System   Research Associate

    2011.10 - 2013.3

  7. Imperial College London   JSPS海外特別研究員

    2010.4 - 2011.9

  8. Tohoku University

    2008.4 - 2010.3

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Education 2

  1. Tohoku University

    2006.4 - 2009.3

  2. Tohoku University

    2004.4 - 2006.3

Professional Memberships 5

  1. THE ELECTROCHEMICAL SOCIETY OF JAPAN

  2. THE BIOPHYSICAL SOCIETY OF JAPAN

  3. THE CHEMICAL SOCIETY OF JAPAN

  4. THE JAPAN SOCIETY FOR ANALYTICAL CHEMISTRY

  5. THE JAPAN SOCIETY OF APPLIED PHYSICS

Awards 20

  1. 2022堀場雅夫賞

    2022.10   触媒活性サイトの実空間イメージングに資する 電気化学セル顕微鏡の開発

  2. 第16回わかしゃち奨励賞

    2022.1   愛知県経済産業局産業部産業科学技術課   ウィルスの取り込み過程の可視化に資する新奇プローブ顕微鏡の開発

    高橋康史

  3. 中谷賞奨励賞

    2020.1   公益財団法人中谷医工計測技術振興財団  

  4. 第1回バイオインダストリー奨励賞

    2017.10   超解像度ケミカルイメージングを実現する電気化学顕微鏡の開発

    高橋 康史

  5. 若手優秀発表賞

    2017.6   日本細胞生物学会   非標識・非侵襲でのナノスケールの形状観察を実現する走査型イオンコンダクタンス顕微鏡の開発と応用

    高橋 康史

  6. 第2回若手研究者奨励賞

    2016.12   金沢大学先端科学・イノベーション推進機構協力会  

    高橋 康史

  7. 文部科学大臣賞若手科学者賞

    2016.4   ナノ電気化学顕微鏡の創製と固液界面計測に関する研究

    高橋 康史

  8. 進歩賞・佐野賞

    2016.3   電気化学会  

  9. 進歩賞・佐野賞

    2016.3   電気化学会   ナノスケールの固液界面計測を実現するナノ電気化学顕微鏡の創成

    高橋 康史

  10. 奨励賞

    2015.9   日本分析化学会  

    高橋 康史

  11. 若手奨励賞

    2015.9   日本生物物理学会   ナノスケールの形状・化学物質濃度プロファイルを可視化するナノ電気化学顕微鏡の創成

    高橋 康史

  12. ナノプローブ奨励賞

    2015.5   JSPS167委員会  

  13. 講演奨励賞

    2015.5   日本化学会  

    高橋 康史

  14. ナノプローブ奨励賞

    2015.5   JSPS167委員会  

    高橋 康史

  15. 第37回内藤コンファレンスポスター賞

    2014.7  

    高橋 康史

  16. 第19回青葉工学研究奨励賞

    2013.12  

    高橋 康史

  17. R&D Encouragement Award

    2013.11   NF Foundation  

    高橋 康史

  18. 総長賞

    2009.3   東北大学  

  19. 総長賞

    2009.3   東北大学  

    高橋 康史

  20. 講演奨励賞

    2004.5   応用物理学会  

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Papers 139

  1. Nanoscrolls of Janus Monolayer Transition Metal Dichalcogenides. International journal

    Masahiko Kaneda, Wenjin Zhang, Zheng Liu, Yanlin Gao, Mina Maruyama, Yusuke Nakanishi, Hiroshi Nakajo, Soma Aoki, Kota Honda, Tomoya Ogawa, Kazuki Hashimoto, Takahiko Endo, Kohei Aso, Tongmin Chen, Yoshifumi Oshima, Yukiko Yamada-Takamura, Yasufumi Takahashi, Susumu Okada, Toshiaki Kato, Yasumitsu Miyata

    ACS nano   Vol. 18 ( 4 ) page: 2772 - 2781   2024.1

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    Tubular structures of transition metal dichalcogenides (TMDCs) have attracted attention in recent years due to their emergent physical properties, such as the giant bulk photovoltaic effect and chirality-dependent superconductivity. To understand and control these properties, it is highly desirable to develop a sophisticated method to fabricate TMDC tubular structures with smaller diameters and a more uniform crystalline orientation. For this purpose, the rolling up of TMDC monolayers into nanoscrolls is an attractive approach to fabricating such a tubular structure. However, the symmetric atomic arrangement of a monolayer TMDC generally makes its tubular structure energetically unstable due to considerable lattice strain in curved monolayers. Here, we report the fabrication of narrow nanoscrolls by using Janus TMDC monolayers, which have an out-of-plane asymmetric structure. Janus WSSe and MoSSe monolayers were prepared by the plasma-assisted surface atom substitution of WSe2 and MoSe2 monolayers, respectively, and then were rolled by solution treatment. The multilayer tubular structures of Janus nanoscrolls were revealed by scanning transmission electron microscopy observations. Atomic resolution elemental analysis confirmed that the Janus monolayers were rolled up with the Se-side surface on the outside. We found that the present nanoscrolls have the smallest diameter of about 5 nm, which is almost the same as the value predicted by the DFT calculation. The difference in work functions between the S- and Se-side surfaces was measured by Kelvin probe force microscopy, which is in good agreement with the theoretical prediction. Strong interlayer interactions and anisotropic optical responses of the Janus nanoscrolls were also revealed by Raman and photoluminescence spectroscopy.

    DOI: 10.1021/acsnano.3c05681

    PubMed

  2. Electrochemical Nanopipette Sensor for In Vitro/In Vivo Detection of Cu2+ Ions. International journal

    Roman V Timoshenko, Petr V Gorelkin, Alexander N Vaneev, Olga O Krasnovskaya, Roman A Akasov, Anastasiia S Garanina, Dmitry A Khochenkov, Tamara M Iakimova, Natalia L Klyachko, Tatiana O Abakumova, Vera S Shashkovskaya, Kirill D Chaprov, Alexander A Makarov, Vladimir A Mitkevich, Yasufumi Takahashi, Christopher R W Edwards, Yuri E Korchev, Alexander S Erofeev

    Analytical chemistry   Vol. 96 ( 1 ) page: 127 - 136   2024.1

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    In vitro/in vivo detection of copper ions is a challenging task but one which is important in the development of new approaches to the diagnosis and treatment of cancer and hereditary diseases such as Alzheimer's, Wilson's, etc. In this paper, we present a nanopipette sensor capable of measuring Cu2+ ions with a linear range from 0.1 to 10 μM in vitro and in vivo. Using the gold-modified nanopipette sensor with a copper chelating ligand, we evaluated the accumulation ability of the liposomal form of an anticancer Cu-containing complex at three levels of biological organization. First, we detected Cu2+ ions in a single cell model of human breast adenocarcinoma MCF-7 and in murine melanoma B16 cells. The insertion of the nanoelectrode did not result in leakage of the cell membrane. We then evaluated the distribution of the Cu-complex in MCF-7 tumor spheroids and found that the diffusion-limited accumulation was a function of the depth, typical for 3D culture. Finally, we demonstrated the use of the sensor for Cu2+ ion detection in the brain of an APP/PS1 transgenic mouse model of Alzheimer's disease and tumor-bearing mice in response to injection (2 mg kg-1) of the liposomal form of the anticancer Cu-containing complex. Enhanced stability and selectivity, as well as distinct copper oxidation peaks, confirmed that the developed sensor is a promising tool for testing various types of biological systems. In summary, this research has demonstrated a minimally invasive electrochemical technique with high temporal resolution that can be used for the study of metabolism of copper or copper-based drugs in vitro and in vivo.

    DOI: 10.1021/acs.analchem.3c03337

    PubMed

  3. In situ visualization of LbL-assembled film nanoscale morphology using scanning ion conductance microscopy

    Kota Honda, Kentaro Yoshida, Katsuhiko Sato, Hiroki Ida, Yasufumi Takahashi

    Electrochimica Acta   Vol. 469   page: 143152 - 143152   2023.11

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    Publishing type:Research paper (scientific journal)   Publisher:Elsevier BV  

    DOI: 10.1016/j.electacta.2023.143152

  4. Electrochemical imaging correlated to hydrogen evolution reaction on transition metal dichalcogenide, WS2

    Akichika Kumatani, Hiroto Ogawa, Takahiko Endo, Yu Kobayashi, Jana Lustikova, Hiroki Ida, Yasufumi Takahashi, Tomokazu Matsue, Yasumitsu Miyata, Hitoshi Shiku

    Journal of Vacuum Science & Technology B     2023.9

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    DOI: 10.1116/6.0002706

  5. Nanopipette Fabrication Guidelines for SICM Nanoscale Imaging. International journal

    Yasufumi Takahashi, Yuya Sasaki, Takeshi Yoshida, Kota Honda, Yuanshu Zhou, Takafumi Miyamoto, Tomoko Motoo, Hiroki Higashi, Andrew Shevchuk, Yuri Korchev, Hiroki Ida, Rikinari Hanayama, Takeshi Fukuma

    Analytical chemistry   Vol. 95 ( 34 ) page: 12664 - 12672   2023.8

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    Scanning ion conductance microscopy (SICM) is a promising tool for visualizing the dynamics of nanoscale cell surface topography. However, there are still no guidelines for fabricating nanopipettes with ideal shape consisting of small apertures and thin glass walls. Therefore, most of the SICM imaging has been at a standstill at the submicron scale. In this study, we established a simple and highly reproducible method for the fabrication of nanopipettes with sub-20 nm apertures. To validate the improvement in the spatial resolution, we performed time-lapse imaging of the formation and disappearance of endocytic pits as a model of nanoscale time-lapse topographic imaging. We have also successfully imaged the localization of the hot spot and the released extracellular vesicles. The nanopipette fabrication guidelines for the SICM nanoscale topographic imaging can be an essential tool for understanding cell-cell communication.

    DOI: 10.1021/acs.analchem.3c01010

    PubMed

  6. Highly sensitive glucose electrochemical sensor using sugar‐lectin interactions

    Kyoko Sugiyama, Fumiya Sato, Sachiko Komatsu, Toshio Kamijo, Kentaro Yoshida, Yusuke Kawabe, Hiromi Nishikawa, Tsutomu Fujimura, Yasufumi Takahashi, Katsuhiko Sato

    Electrochemical Science Advances     2023.7

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    Publishing type:Research paper (scientific journal)   Publisher:Wiley  

    DOI: 10.1002/elsa.202300015

  7. Electrodeposited Gold Probe for Electrochemical Scanning Tunneling Microscopy

    Yuzu Kobayashi, Yasuyuki Yokota, Yasufumi Takahashi, Jun Takeya, Yousoo Kim

    The Journal of Physical Chemistry C   Vol. 127 ( 28 ) page: 13929 - 13935   2023.7

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    Publishing type:Research paper (scientific journal)   Publisher:American Chemical Society (ACS)  

    DOI: 10.1021/acs.jpcc.3c02690

  8. 1T/1H-SnS2 Sheets for Electrochemical CO2 Reduction to Formate. International journal

    Yusuke Kawabe, Yoshikazu Ito, Yuta Hori, Suresh Kukunuri, Fumiya Shiokawa, Tomohiko Nishiuchi, Samuel Jeong, Kosuke Katagiri, Zeyu Xi, Zhikai Li, Yasuteru Shigeta, Yasufumi Takahashi

    ACS nano   Vol. 17 ( 12 ) page: 11318 - 11326   2023.6

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    Understanding the catalytic mechanism of highly active two-dimensional electrocatalysts is crucial to their rational design. Herein, we reveal the element dependence of the reactivity of two-dimensional metal dichalcogenide sheets for electrocatalytic CO2 reduction. We found that tin(IV) disulfide (SnS2) and molybdenum(IV) disulfide (MoS2) sheets exhibited Faradaic efficiencies of 63.3% and ∼0%, respectively, for formic acid. Scanning electrochemical cell microscopy and theoretical calculations were used to identify the catalytically active sites of SnS2 as terraces and edges. Owing to the effective utilization of the entire surface area, SnS2 can effectively accelerate catalytic reactions. This finding provides a direction for material research in two-dimensional electrocatalysts for energy-efficient chemical production from electrochemical CO2 reduction, as well as for other energy devices.

    DOI: 10.1021/acsnano.2c12627

    PubMed

  9. Topographical evaluation of human mesenchymal stem cells during osteogenic differentiation using scanning ion conductance microscopy Reviewed

    Kota Nozawa, Xuyang Zhang, Takuo Nakamura, Yuji Nashimoto, Yasufumi Takahashi, Kosuke Ino, Hitoshi Shiku

    Electrochimica Acta     2023.3

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    Language:English   Publishing type:Research paper (scientific journal)  

    DOI: 10.1016/j.electacta.2023.142192

  10. Surface morphology live-cell imaging reveals how macropinocytosis inhibitors affect membrane dynamics

    Hiroki Ida, Noriko Taira, Koichi Azuma, Akichika Kumatani, Misao Akishiba, Shiroh Futaki, Yasufumi Takahashi, Hitoshi Shiku

    Electrochimica Acta   Vol. 441   page: 141783 - 141783   2023.2

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    Publishing type:Research paper (scientific journal)   Publisher:Elsevier BV  

    DOI: 10.1016/j.electacta.2022.141783

    Web of Science

  11. Correlative Analysis of Ion-Concentration Profile and Surface Nanoscale Topography Changes Using Operando Scanning Ion Conductance Microscopy Reviewed International journal

    Yasufumi Takahashi, Daiko Takamatsu, Yuri Korchev, Takeshi Fukuma

    JACS AU   Vol. 3 ( 4 ) page: 1089 - 1099   2023.2

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    Language:English   Publishing type:Research paper (scientific journal)   Publisher:AMER CHEMICAL SOC  

    Although various spectroscopic methods have been developed to capture ion-concentration profile changes, it is still difficult to visualize the ion-concentration profile and surface topographical changes simultaneously during the charging/ discharging of lithium-ion batteries (LIBs). To tackle this issue, we have developed an operando scanning ion conductance microscopy (SICM) method that can directly visualize an ion concentration profile and surface topography using a SICM nanopipette while controlling the sample potential or current with a potentiostat for characterizing the polarization state during charging/discharging. Using operando SICM on the negative electrode (anode) of LIBs, we have characterized ion-concentration profile changes and the reversible volume changes related to the phase transition during cyclic voltammetry (CV) and charge/ discharge of the graphite anode. Operando SICM is a versatile technique that is likely to be of major value for evaluating the correlation between the electrolyte concentration profile and nanoscale surface topography changes.

    DOI: 10.1021/jacsau.2c00677

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  12. Vancomycin sensing using a phenylboronic acid-modified nanopore pipette

    Fumiya Sato, Haruka Nakano, Toshio Kamijo, Kazuhiro Watanabe, Tsutomu Fujimura, Yasufumi Takahashi, Katsuhiko Sato

    Electroanalysis     2023

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    Nanopore sensing measures the changes in charge and physical state around the nanopores as changes in ionic current. In this study, we performed vancomycin (VCM) sensing with nanopores modified via Au−S bonds with dithiobis(4-butyrylamino-m-phenylboronic acid) (DTBA-PBA), a derivative of phenylboronic acid (PBA) bearing a thiol. First, we modified a 3-mm-diameter Au electrode with a DTBA-PBA self-assembled monolayer (SAM) to confirm the VCM response of the PBA interface by cyclic voltammetry. DTBA-PBA was then immobilized in the same manner on a nanopore pipette coated with an Au layer. We measured the VCM concentration from the change in ion current using the nanopore pipette. A VCM concentration-dependent ionic current response was observed in the range of 0.01–1 mM. Many kinds of pharmaceuticals can bind to PBA; therefore, this method could be used for quick, easy, in situ quantification of not only VCM but also other pharmaceuticals with serious side effects.

    DOI: 10.1002/elan.202300173

    Scopus

  13. A noncanonical endocytic pathway is involved in the internalization of 3 μm polystyrene beads into HeLa cells. International journal

    Hisaaki Hirose, Masashi Maekawa, Hiroki Ida, Masashi Kuriyama, Yasufumi Takahashi, Shiroh Futaki

    Biomaterials science   Vol. 10 ( 24 ) page: 7093 - 7102   2022.12

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    Extracellular fine particles of various sizes and origins can be taken up by cells, affecting their function. Understanding the cellular uptake processes is crucial for understanding the cellular effects of these particles and the development of means to control their internalization. Although macropinocytosis is a possible pathway for the cellular uptake of particles larger than 0.2 μm, its contribution to cellular uptake in non-phagocytic cells is controversial. Using 3 μm polystyrene beads as a model particle, we aimed to assess the detailed modes of their cellular uptake by non-phagocytic HeLa cells. Cellular uptake was assessed using confocal, scanning electron, and scanning ion conductance microscopy analyses, together with inhibitor studies. Our results revealed that 3 μm beads were taken up by HeLa cells by an actin-, cholesterol-, and membrane protrusions-dependent noncanonical endocytic pathway, different from the canonical macropinocytic and phagocytic pathways. Our work provides a framework for studying the cellular uptake of extracellular fine particles.

    DOI: 10.1039/d2bm01353c

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    PubMed

  14. Autotuning of Vibrational Strong Coupling for Site-Selective Reactions. International journal

    Kenji Hirai, Hiroto Ishikawa, Yasufumi Takahashi, James Andell Hutchison, Hiroshi Uji-I

    Chemistry (Weinheim an der Bergstrasse, Germany)   Vol. 28 ( 47 ) page: e202201260   2022.5

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    Site-selective chemistry opens new paths for the synthesis of technologically important molecules. When a reactant is placed inside a Fabry-Perot (FP) cavity, energy exchange between molecular vibrations and resonant cavity photons results in vibrational strong coupling (VSC). VSC has recently been implicated in modified chemical reactivity at specific reactive sites. However, as a reaction proceeds inside an FP cavity, the refractive index of the reaction solution changes, detuning the cavity mode away from the vibrational mode and weakening the VSC effect. Here we overcome this issue, developing actuatable FP cavities to allow automated tuning of cavity mode energy to maintain maximized VSC during a reaction. As an example, the site-selective reaction of the aldehyde over the ketone in 4-acetylbenzaldehyde is achieved by automated cavity tuning to maintain optimal VSC of the ketone carbonyl stretch during the reaction. A nearly 50% improvement in site-selective reactivity is observed compared to an FP cavity with static mirrors, demonstrating the utility of actuatable FP cavities as microreactors for organic chemistry.

    DOI: 10.1002/chem.202201260

    PubMed

  15. In Vitro/In Vivo Electrochemical Detection of Pt(II) Species. International journal

    Alexander N Vaneev, Petr V Gorelkin, Olga O Krasnovskaya, Roman A Akasov, Daniil V Spector, Elena V Lopatukhina, Roman V Timoshenko, Anastasiia S Garanina, Yanjun Zhang, Sergey V Salikhov, Christopher R W Edwards, Natalia L Klyachko, Yasufumi Takahashi, Alexander G Majouga, Yuri E Korchev, Alexander S Erofeev

    Analytical chemistry   Vol. 94 ( 12 ) page: 4901 - 4905   2022.3

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    The biodistribution of chemotherapy compounds within tumor tissue is one of the main challenges in the development of antineoplastic drugs, and techniques for simple, inexpensive, sensitive, and selective detection of various analytes in tumors are of great importance. In this paper we propose the use of platinized carbon nanoelectrodes (PtNEs) for the electrochemical detection of platinum-based drugs in various biological models, including single cells and tumor spheroids in vitro and inside solid tumors in vivo. We have demonstrated the quantitative direct detection of Pt(II) in breast adenocarcinoma MCF-7 cells treated with cisplatin and a cisplatin-based DNP prodrug. To realize the potential of this technique in advanced tumor models, we measured Pt(II) in 3D tumor spheroids in vitro and in tumor-bearing mice in vivo. The concentration gradient of Pt(II) species correlated with the distance from the sample surface in MCF-7 tumor spheroids. We then performed the detection of Pt(II) species in tumor-bearing mice treated intravenously with cisplatin and DNP. We found that there was deeper penetration of DNP in comparison to cisplatin. This research demonstrates a minimally invasive, real-time electrochemical technique for the study of platinum-based drugs.

    DOI: 10.1021/acs.analchem.2c00136

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  16. Alkaline Phosphatase-based Electrochemical Analysis for Point-of-Care Testing

    Yusuke Kanno, Yuanshu Zhou, Takeshi Fukuma, Yasufumi Takahashi

    Electroanalysis   Vol. 34 ( 2 ) page: 161 - 167   2022.2

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    Point-of-care testing (POCT) devices have evolved to provide beneficial information about an individual's health whenever needed. Enzyme-based analytical devices have facilitated the highly selective detection of numerous biological molecules and ions. Enzymes are commonly used as the tags of recognition components, such as antibodies, to generate and amplify detection signals. Particularly, alkaline phosphatase (ALP) is one of the most widely used enzymes because of its high turnover number and low cost. Rapid response time and the incorporation of many sensors fabricated by micro/nano processing technologies are the advantages in using electrochemical devices as analytical tools. Therefore, ALP-based electrochemical devices have potential applications for more practical POCT platforms. This review summarizes recent research progress of ALP-based electrochemical devices for POCT. In addition to ALP substrates, the application of ALP-based immunosensors, aptasensors, and DNAzyme sensors are discussed.

    DOI: 10.1002/elan.202100294

    Scopus

  17. Direct Electrochemical Visualization of the Orthogonal Charge Separation in Anatase Nanotube Photoanodes for Water Splitting

    Marina V. Makarova, Fumiaki Amano, Shinpei Nomura, Chihiro Tateishi, Takeshi Fukuma, Yasufumi Takahashi, Yuri E. Korchev

    ACS Catalysis   Vol. 12 ( 2 ) page: 1201 - 1208   2022.1

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    Language:Japanese   Publishing type:Research paper (scientific journal)  

    Photoelectrochemical (PEC) water splitting is an important and rapidly developing technology that produces H2 as a renewable resource, but local surface investigations remain a major challenge. Using scanning electrochemical cell microscopy (SECCM), the PEC catalytic effects of anatase TiO2-nanotube arrays grown on Ti felt are explored. The SECCM imaging is performed both perpendicular and parallel to the nanotube growth direction. In contrast to bulk cyclic voltammetry measurements, SECCM measures only the upper region of the nanotubes that remain in contact with the electrolyte, which provides a better understanding of the phenomena connected to the longitudinal charge transport. Despite the presence of regions with higher and lower photocurrent, the PEC reactivities of the nanotube tops and walls are roughly comparable with each other. The data support the model of orthogonal electron-hole separation. This model facilitates the photogenerated hole diffusion over the short distance to the electrolyte interface due to the sufficient transport of photoexcited electrons along the long axial direction of TiO2 nanotubes and is often applied to one-dimensional systems. Observed results were additionally supported by the nanotube decoration with photoelectrochemically deposited PbO2 particles.

    DOI: 10.1021/acscatal.1c04910

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  18. Characterization of the Depth of Discharge-Dependent Charge Transfer Resistance of a Single LiFePO4 Particle. International journal

    Takahiko Yamamoto, Tomohiro Ando, Yusuke Kawabe, Takeshi Fukuma, Hiroshi Enomoto, Yoshiaki Nishijima, Yoshihiko Matsui, Kiyoshi Kanamura, Yasufumi Takahashi

    Analytical chemistry   Vol. 93 ( 43 ) page: 14448 - 14453   2021.11

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    The discharged state affects the charge transfer resistance of lithium-ion secondary batteries (LIBs), which is referred to as the depth of discharge (DOD). To understand the intrinsic charge/discharge property of LIBs, the DOD-dependent charge transfer resistance at the solid-liquid interface is required. However, in a general composite electrode, the conductive additive and organic polymeric binder are unevenly distributed, resulting in a complicated electron conduction/ion conduction path. As a result, estimating the DOD-dependent rate-determining factor of LIBs is difficult. In contrast, in micro/nanoscale electrochemical measurements, the primary or secondary particle is evaluated without using a conductive additive and providing an ideal mass transport condition. To control the DOD state of a single LiFePO4 active material and evaluate the DOD-dependent charge transfer kinetic parameters, we use scanning electrochemical cell microscopy (SECCM), which uses a micropipette to form an electrochemical cell on a sample surface. The difference in charge transfer resistance at the solid-liquid interface depending on the DOD state and electrolyte solution could be confirmed using SECCM.

    DOI: 10.1021/acs.analchem.1c02851

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  19. Scanning electrochemical microscopy for biosurface imaging

    Yuanshu Zhou, Yasufumi Takahashi, Takeshi Fukuma, Tomokazu Matsue

    Current Opinion in Electrochemistry   Vol. 29   page: 100739 - 100739   2021.10

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    Language:Japanese   Publishing type:Research paper (scientific journal)   Publisher:Elsevier BV  

    DOI: 10.1016/j.coelec.2021.100739

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  20. Topography and Permeability Analyses of Vasculature-on-a-Chip Using Scanning Probe Microscopies. International journal

    Yuji Nashimoto, Minori Abe, Ryota Fujii, Noriko Taira, Hiroki Ida, Yasufumi Takahashi, Kosuke Ino, Javier Ramon-Azcon, Hitoshi Shiku

    Advanced healthcare materials   Vol. 10 ( 21 ) page: e2101186   2021.8

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    Microphysiological systems (MPS) or organs-on-chips (OoC) can emulate the physiological functions of organs in vitro and are effective tools for determining human drug responses in preclinical studies. However, the analysis of MPS has relied heavily on optical tools, resulting in difficulties in real-time and high spatial resolution imaging of the target cell functions. In this study, the role of scanning probe microscopy (SPM) as an analytical tool for MPS is evaluated. An access hole is made in a typical MPS system with stacked microchannels to insert SPM probes into the system. For the first study, a simple vascular model composed of only endothelial cells is prepared for SPM analysis. Changes in permeability and local chemical flux are quantitatively evaluated during the construction of the vascular system. The morphological changes in the endothelial cells after flow stimulation are imaged at the single-cell level for topographical analysis. Finally, the possibility of adapting the permeability and topographical analysis using SPM for the intestinal vascular system is further evaluated. It is believed that this study will pave the way for an in situ permeability assay and structural analysis of MPS using SPM.

    DOI: 10.1002/adhm.202101186

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  21. Geometric model of 3D curved graphene with chemical dopants

    Andreas Dechant, Tatsuhiko Ohto, Yoshikazu Ito, Marina V. Makarova, Yusuke Kawabe, Tatsufumi Agari, Hikaru Kumai, Yasufumi Takahashi, Hisashi Naito, Motoko Kotani

    Carbon   Vol. 182   page: 223 - 232   2021.6

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    Language:Japanese   Publishing type:Research paper (scientific journal)   Publisher:Elsevier BV  

    DOI: 10.1016/j.carbon.2021.06.004

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  22. Nanoscale characterization of the site‐specific degradation of electric double‐layer capacitor using scanning electrochemical cell microscopy

    Yusuke Kawabe, Yosuke Miyakoshi, Rui Tang, Takeshi Fukuma, Hirotomo Nishihara, Yasufumi Takahashi

    Electrochemical Science Advances   Vol. 2 ( 3 )   2021.5

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    Publishing type:Research paper (scientific journal)   Publisher:Wiley  

    DOI: 10.1002/elsa.202100053

    Other Link: https://onlinelibrary.wiley.com/doi/full-xml/10.1002/elsa.202100053

  23. Nanoscale Reactivity Mapping of a Single-Crystal Boron-Doped Diamond Particle. International journal

    Tomohiro Ando, Kai Asai, Julie Macpherson, Yasuaki Einaga, Takeshi Fukuma, Yasufumi Takahashi

    Analytical chemistry   Vol. 93 ( 14 ) page: 5831 - 5838   2021.4

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    Boron-doped diamond (BDD) is most often grown by chemical vapor deposition (CVD) in polycrystalline form, where the electrochemical response is averaged over the whole surface. Deconvoluting the impact of crystal orientation, surface termination, and boron-doped concentration on the electrochemical response is extremely challenging. To tackle this problem, we use CVD to grow isolated single-crystal microparticles of BDD with the crystal facets (100, square-shaped) and (111, triangle-shaped) exposed and combine with hopping mode scanning electrochemical cell microscopy (HM-SECCM) for electrochemical interrogation of the individual crystal faces (planar and nonplanar). Measurements are made on both hydrogen- (H-) and oxygen (O-)-terminated single-crystal facets with two different redox mediators, [Ru(NH3)6]3+/2+ and Fe(CN)64-/3-. Extraction of the half-wave potential from linear sweep and cyclic voltammetric experiments at all measurement (pixel) points shows unequivocally that electron transfer is faster at the H-terminated (111) surface than at the H-terminated (100) face, attributed to boron dopant differences. The most dramatic differences were seen for [Ru(NH3)6]3+/2+ when comparing the O-terminated (100) surface to the H-terminated (100) face. Removal of the H-surface conductivity layer and a potential-dependent density of states were thought to be responsible for the behavior observed. Finally, a bimodal distribution in the electrochemical activity on the as-grown H-terminated polycrystalline BDD electrode is attributed to the dominance of differently doped (100) and (111) facets in the material.

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  24. Mapping mechanical properties of living cells at nanoscale using intrinsic nanopipette-sample force interactions. International journal

    Vasilii S Kolmogorov, Alexander S Erofeev, Emily Woodcock, Yuri M Efremov, Aleksei P Iakovlev, Nikita A Savin, Anna V Alova, Svetlana V Lavrushkina, Igor I Kireev, Alexandra O Prelovskaya, Elena V Sviderskaya, Denis Scaini, Natalia L Klyachko, Peter S Timashev, Yasufumi Takahashi, Sergey V Salikhov, Yuri N Parkhomenko, Alexander G Majouga, Christopher R W Edwards, Pavel Novak, Yuri E Korchev, Petr V Gorelkin

    Nanoscale   Vol. 13 ( 13 ) page: 6558 - 6568   2021.4

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    Mechanical properties of living cells determined by cytoskeletal elements play a crucial role in a wide range of biological functions. However, low-stress mapping of mechanical properties with nanoscale resolution but with a minimal effect on the fragile structure of cells remains difficult. Scanning Ion-Conductance Microscopy (SICM) for quantitative nanomechanical mapping (QNM) is based on intrinsic force interactions between nanopipettes and samples and has been previously suggested as a promising alternative to conventional techniques. In this work, we have provided an alternative estimation of intrinsic force and stress and demonstrated the possibility to perform qualitative and quantitative analysis of cell nanomechanical properties of a variety of living cells. Force estimation on decane droplets with well-known elastic properties, similar to living cells, revealed that the forces applied using a nanopipette are much smaller than in the case using atomic force microscopy. We have shown that we can perform nanoscale topography and QNM using a scanning procedure with no detectable effect on live cells, allowing long-term QNM as well as detection of nanomechanical properties under drug-induced alterations of actin filaments and microtubulin.

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  25. Nanoscale Visualization of Morphological Alteration of Live-Cell Membranes by the Interaction with Oligoarginine Cell-Penetrating Peptides. International journal

    Hiroki Ida, Yasufumi Takahashi, Akichika Kumatani, Hitoshi Shiku, Tomo Murayama, Hisaaki Hirose, Shiroh Futaki, Tomokazu Matsue

    Analytical chemistry   Vol. 93 ( 13 ) page: 5383 - 5393   2021.4

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    The interactions between the cell membrane and biomolecules remain poorly understood. For example, arginine-rich cell-penetrating peptides (CPPs), including octaarginines (R8), are internalized by interactions with cell membranes. However, during the internalization process, the exact membrane dynamics introduced by these CPPs are still unknown. Here, we visualize arginine-rich CPPs and cell-membrane interaction-induced morphological changes using a system that combines scanning ion-conductance microscopy and spinning-disk confocal microscopy, using fluorescently labeled R8. This system allows time-dependent, nanoscale visualization of structural dynamics in live-cell membranes. Various types of membrane remodeling caused by arginine-rich CPPs are thus observed. The induction of membrane ruffling and the cup closure are observed as a process of endocytic uptake of the peptide. Alternatively suggested is the concave structural formation accompanied by direct peptide translocation through cell membranes. Studies using R8 without fluorescent labeling also demonstrate a non-negligible effect of the fluorescent moiety on membrane structural alteration.

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  26. Micropipet-Based Navigation in a Microvascular Model for Imaging Endothelial Cell Topography Using Scanning Ion Conductance Microscopy. International journal

    Noriko Taira, Yuji Nashimoto, Kosuke Ino, Hiroki Ida, Takuto Imaizumi, Akichika Kumatani, Yasufumi Takahashi, Hitoshi Shiku

    Analytical chemistry   Vol. 93 ( 11 ) page: 4902 - 4908   2021.3

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    Scanning ion conductance microscopy (SICM) has enabled cell surface topography at a high resolution with low invasiveness. However, SICM has not been applied to the observation of cell surfaces in hydrogels, which can serve as scaffolds for three-dimensional cell culture. In this study, we applied SICM for imaging a cell surface in a microvascular lumen reconstructed in a hydrogel. To achieve this goal, we developed a micropipet navigation technique using ionic current to detect the position of a microvascular lumen. Combining this navigation technique with SICM, endothelial cells in a microvascular model and blebs were visualized successfully at the single-cell level. To the best of our knowledge, this is the first report on visualizing cell surfaces in hydrogels using a SICM. This technique will be useful for furthering our understanding of the mechanism of intravascular diseases.

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  27. Electrochemical Imaging of a Single Crystal Boron-doped Diamond

    Kawabe Yusuke, Ando Tomohiro, Asai Kai, Tomisaki Mai, Einaga Yasuaki, Fukuma Takeshi, Takahashi Yasufumi

    JSAP Annual Meetings Extended Abstracts   Vol. 2021.1 ( 0 ) page: 1370 - 1370   2021.2

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    DOI: 10.11470/jsapmeeting.2021.1.0_1370

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  28. Acceleration of Electrochemical CO<inf>2</inf>Reduction to Formate at the Sn/Reduced Graphene Oxide Interface

    Takuya Tsujiguchi, Yusuke Kawabe, Samuel Jeong, Tatsuhiko Ohto, Suresh Kukunuri, Hirotaka Kuramochi, Yasufumi Takahashi, Tomohiko Nishiuchi, Hideki Masuda, Mitsuru Wakisaka, Kailong Hu, Ganesan Elumalai, Jun Ichi Fujita, Yoshikazu Ito

    ACS Catalysis   Vol. 11 ( 6 ) page: 3310 - 3318   2021

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    Electrochemical CO2 reduction is a key technology to recycle CO2 as a renewable resource, but adsorbing CO2 on the catalyst surface is challenging. We explored the effects of reduced graphene oxide (rGO) in Sn/rGO composites and found that the CO2 adsorption ability of Sn/rGO was almost 4-times higher than that of bare Sn catalysts. Density functional theory calculations revealed that the oxidized functional groups of rGO offered adsorption sites for CO2 toward the adjacent Sn surface and that CO2-rich conditions near the surface facilitated the production of formate via COOH∗ formation while suppressing CO∗ formation. Scanning electrochemical cell microscopy directly indicated that CO2 reduction was accelerated at the interface, together with the kinetic suppression of undesirable and competitive hydrogen evolution at the interface. Thus, the synergism of Sn/rGO ensures a substantial/rapid supply of CO2 from the functional groups to the Sn surface, thereby enhancing the Faradaic efficiency 1.8-times compared with that obtained with bare Sn catalysts.

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  29. Microelectrode-based transient amperometry of O2 adsorption and desorption on a SrTiO3 photocatalyst excited under water International journal

    Takumu Kosaka, Tomohiro Ando, Takashi Hisatomi, Hiroshi Nishiyama, Yuanshu Zhou, Kazunari Domen, Yasufumi Takahashi, Hiroshi Onishi

    Physical Chemistry Chemical Physics   Vol. 23 ( 35 ) page: 19386 - 19393   2021

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    Transient amperometry with a microelectrode was applied to a SrTiO<sub>3</sub> photocatalyst for water splitting. <italic>Operando</italic> O<sub>2</sub> detection at intervals of 0.1 s indicated light-triggered O<sub>2</sub> adsorption and desorption in addition to photocatalytic O<sub>2</sub> evolution.

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  30. Electrochemical Quantitative Evaluation of the Surface Charge of a Poly(1-vinylimidazole) Multilayer Film and Application to Nanopore pH Sensor

    Katsuhiko Sato, Fumiya Sato, Masayuki Kumano, Toshio Kamijo, Takaya Sato, Yuanshu Zhou, Yuri Korchev, Takeshi Fukuma, Tsutomu Fujimura, Yasufumi Takahashi

    Electroanalysis   Vol. 33 ( 6 ) page: 1633 - 1638   2021

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    Nanopore pH sensing is based on the interaction between the surface charge of the nanopore and ions passing through the nanopore. The nanopore surface charge can be derived from the acid-base dissociation equilibrium of the modified polyelectrolyte. Various polyelectrolytes have been selected based on the acid dissociation constant of the monomer units, and various techniques have been applied to modify nanopores. However, they have been developed without clear guidelines for characterizing the surface modification status or surface charge. One reason has been the difficulty in accurately estimating the surface charge of nanopores in solution. Thus, in this study, the dissociation constant (pKa ) of the surface charge of a modified polyelectrolyte nanopore was quantitatively estimated via electrochemical measurements. Previously, the modification status of nanopores has been evaluated using the ion current response. In addition, we monitored in real-time the polyelectrolyte modification status using a quartz crystal microbalance (QCM). Some polyelectrolytes were difficult to immobilize directly on the nanopore surface, and those polymers could be effectively modified by the layer-by-layer (LbL) technique. Therefore, we produced a guideline for the fabrication of a nanopore sensor for pH measurements under physiological conditions by quantitative evaluation of the pKa via electrochemical methods, the monitoring of the modification status by QCM, and the development of an effective modification method via the LbL technique. app app

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  31. Development of nanoscale electrochemical imaging tool using nanopipette

    Takahashi Yasufumi

    Abstract book of Annual Meeting of the Japan Society of Vacuum and Surface Science   Vol. 2021 ( 0 ) page: 1Da05   2021

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    <p>To improve the performance of catalysts and batteries, it is very important to visualize the surface reactivity with the structure on a micro/nanoscale to understand the crystal orientation and grain boundary-dependent reactivity. Therefore, we have developed scanning electrochemical cell microscopy that uses a nanopipette as a probe to locally form an electrochemical cell and scan the nanopipette on the sample surface to visualize the reactivity of the sample surface. Using SECCM, we characterized the hydrogen evolution reaction of nanosheet material and the charge/discharge property of the lithium-ion secondary battery.</p>

    DOI: 10.14886/jvss.2021.0_1da05

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  32. Transient Kinetics of O<inf>2</inf>Evolution in Photocatalytic Water-Splitting Reaction

    Takumu Kosaka, Yuya Teduka, Takuya Ogura, Yuanshu Zhou, Takashi Hisatomi, Hiroshi Nishiyama, Kazunari Domen, Yasufumi Takahashi, Hiroshi Onishi

    ACS Catalysis   Vol. 10 ( 22 ) page: 13159 - 13164   2020.11

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    © Water splitting to produce H2 and O2 is a fundamental reaction for artificial photosynthesis on semiconductor photocatalysts. The mechanism of the multistepped reaction, especially four-electron oxidation to O2, has not yet been understood. Although some intermediate states have been detected in transient spectroscopy, O2 evolution kinetics remain unknown at the end of consecutive reaction steps. We apply operando O2 detection with a microelectrode to determine the absolute evolution rate on a highly efficient SrTiO3 photocatalyst film casted on a glass plate. The evolution rate was determined with a time resolution of 0.1 s, which was improved by 1000 times compared with that in widely used gas-chromatographic detection. The observed rate did not respond instantaneously to excitation light irradiation. When light was turned on, the photocatalyst film was inactive for evolution and light-activated in seconds. It was proposed that the first absorbed photons were consumed to fill trap states on SrTiO3 surface and then the latter photons drove steady O2 evolution. When excitation light stopped, the O2 evolution rate exponentially decayed in seconds. The microelectrode method demonstrated herein will be useful for understanding many other reaction kinetics at liquid-solid interfaces.

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  33. Nanoscale kinetic imaging of lithium ion secondary battery materials using scanning electrochemical cell microscopy. Reviewed International journal

    Yasufumi Takahashi, Tsubasa Yamashita, Daiko Takamatsu, Akichika Kumatani, Takeshi Fukuma

    Chemical communications (Cambridge, England)   Vol. 56 ( 65 ) page: 9324 - 9327   2020.7

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    To visualize the electrochemical reactivity and obtain the diffusion coefficient of the anode of lithium-ion batteries, we used scanning electrochemical cell microscopy (SECCM) in a glovebox. SECCM provided the facet-dependent diffusion coefficient on a Li4Ti5O12 (LTO) thin-film electrode and detected the metastable crystal phase of LixFePO4.

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  34. In Vitro and In Vivo Electrochemical Measurement of Reactive Oxygen Species After Treatment with Anticancer Drugs. Reviewed International journal

    Alexander N Vaneev, Petr V Gorelkin, Anastasiia S Garanina, Helena V Lopatukhina, Stepan S Vodopyanov, Anna V Alova, Oxana O Ryabaya, Roman A Akasov, Yanjun Zhang, Pavel Novak, Sergey V Salikhov, Maxim A Abakumov, Yasufumi Takahashi, Christopher R W Edwards, Natalia L Klyachko, Alexander G Majouga, Yuri E Korchev, Alexander S Erofeev

    Analytical chemistry   Vol. 92 ( 12 ) page: 8010 - 8014   2020.5

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    In vivo monitoring of reactive oxygen species (ROS) in tumors during treatment with anticancer therapy is important for understanding the mechanism of action and in the design of new anticancer drugs. In this work, a platinized nanoelectrode is placed into a single cell for detection of the ROS signal, and drug-induced ROS production is then recorded. The main advantages of this method are the short incubation time with the drug and its high sensitivity which allows the detection of low intracellular ROS concentrations. We have shown that our new method can measure the ROS response to chemotherapy in tumor-bearing mice in real-time. ROS levels were measured in vivo inside the tumor at different depths in response to doxorubicin. This work provides an effective new approach for the measurement of intracellular ROS by platinized nanoelectrodes.

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  35. Confinement of Hydrogen Molecules at Graphene-Metal Interface by Electrochemical Hydrogen Evolution Reaction Reviewed

    Satoshi Yasuda, Kazuhisa Tamura, Tomo O. Terasawa, Masahiro Yano, Hideaki Nakajima, Takahiro Morimoto, Toshiya Okazaki, Ryuushi Agari, Yasufumi Takahashi, Masaru Kato, Ichizo Yagi, Hidehito Asaoka

    Journal of Physical Chemistry C   Vol. 124 ( 9 ) page: 5300 - 5307   2020.3

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    Copyright © 2020 American Chemical Society. Confinement of hydrogen molecules at graphene-substrate interface has presented significant importance from the viewpoints of development of fundamental understanding of two-dimensional material interface and energy storage system. In this study, we investigate H2 confinement at a graphene-Au interface by combining selective proton permeability of graphene and the electrochemical hydrogen evolution reaction (electrochemical HER) method. After HER on a graphene/Au electrode in protonic acidic solution, scanning tunneling microscopy finds that H2 nanobubble structures can be produced between graphene and the Au surface. Defect dependence of the bubble formation suggests that intrinsic defects in graphene, which have high hydrogen permeation barrier but are permeable for protons, are involved in the fundamental mechanism of bubble formation. Strain analysis by Raman spectroscopy also shows that atomic size roughness on the graphene/Au surface originating from the HER-induced strain relaxation of graphene plays significant role in formation of the nucleation site and H2 storage capacity. The result presented herein would provide further understanding of molecular confinement at graphene-based interface and development of novel energy material.

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  36. High-Resolution Electrochemical Mapping of the Hydrogen Evolution Reaction on Transition-Metal Dichalcogenide Nanosheets Reviewed

    Yasufumi Takahashi, Yu Kobayashi, Ziqian Wang, Yoshikazu Ito, Masato Ota, Hiroki Ida, Akichika Kumatani, Keisuke Miyazawa, Takeshi Fujita, Hitoshi Shiku, Yuri E. Korchev, Yasumitsu Miyata, Takeshi Fukuma, Mingwei Chen, Tomokazu Matsue

    Angewandte Chemie - International Edition   Vol. 59 ( 9 ) page: 3601 - 3608   2020.2

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    © 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim High-resolution scanning electrochemical cell microscopy (SECCM) is used to image and quantitatively analyze the hydrogen evolution reaction (HER) catalytically active sites of 1H-MoS2 nanosheets, MoS2, and WS2 heteronanosheets. Using a 20 nm radius nanopipette and hopping mode scanning, the resolution of SECCM was beyond the optical microscopy limit and visualized a small triangular MoS2 nanosheet with a side length of ca. 130 nm. The electrochemical cell provides local cyclic voltammograms with a nanoscale spatial resolution for visualizing HER active sites as electrochemical images. The HER activity difference of edge, terrace, and heterojunction of MoS2 and WS2 were revealed. The SECCM imaging directly visualized the relationship of HER activity and number of MoS2 nanosheet layers and unveiled the heterogeneous aging state of MoS2 nanosheets. SECCM can be used for improving local HER activities by producing sulfur vacancies using electrochemical reaction at the selected region.

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  37. High-Speed SICM for the Visualization of Nanoscale Dynamic Structural Changes in Hippocampal Neurons. Reviewed International journal

    Yasufumi Takahashi, Yuanshu Zhou, Takafumi Miyamoto, Hiroki Higashi, Noritaka Nakamichi, Yuka Takeda, Yukio Kato, Yuri Korchev, Takeshi Fukuma

    Analytical chemistry   Vol. 92 ( 2 ) page: 2159 - 2167   2020.1

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    Dynamic reassembly of the cytoskeleton and structural changes represented by dendritic spines, cargo transport, and synapse formation are closely related to memory. However, the visualization of the nanoscale topography is challenging because of the diffraction limit of optical microscopy. Scanning ion conductance microscopy (SICM) is an effective tool for visualizing the nanoscale topography changes of the cell surface without labeling. The temporal resolution of SICM is a critical issue of live-cell time-lapse imaging. Here, we developed a new scanning method, automation region of interest (AR)-mode SICM, to select the next imaging region by predicting the location of a cell, thus improving the scanning speed of time-lapse imaging. The newly developed algorithm reduced the scanning time by half. The time-lapse images provided not only novel information about nanoscale structural changes but also quantitative information on the dendritic spine and synaptic bouton volume changes and formation process of the neural network that are closely related to memory. Furthermore, translocation of plasmalemmal precursor vesicles (ppvs), for which fluorescent labeling has not been established, were also visualized along with the rearrangement of the cytoskeleton at the growth cone.

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  38. Development and application of scanning electrochemical cell microscope for electrochemical imaging of catalytic active sites

    TAKAHASHI Yasufumi, ITO Yoshikazu, KUMATANI Akichika, IDA Hiroki, MIYATA Yasumitsu, MATSUE Tomokazu, FUKUMA Takeshi

    Denki Kagaku   Vol. 88 ( 3 ) page: 229 - 234   2020

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  39. High-resolution label-free 3D mapping of extracellular pH of single living cells. Reviewed International journal

    Zhang Y, Takahashi Y, Hong SP, Liu F, Bednarska J, Goff PS, Novak P, Shevchuk A, Gopal S, Barozzi I, Magnani L, Sakai H, Suguru Y, Fujii T, Erofeev A, Gorelkin P, Majouga A, Weiss DJ, Edwards C, Ivanov AP, Klenerman D, Sviderskaya EV, Edel JB, Korchev Y

    Nature communications   Vol. 10 ( 1 ) page: 5610 - 5610   2019.12

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    Dynamic mapping of extracellular pH (pHe) at the single-cell level is critical for understanding the role of H+ in cellular and subcellular processes, with particular importance in cancer. While several pHe sensing techniques have been developed, accessing this information at the single-cell level requires improvement in sensitivity, spatial and temporal resolution. We report on a zwitterionic label-free pH nanoprobe that addresses these long-standing challenges. The probe has a sensitivity > 0.01 units, 2 ms response time, and 50 nm spatial resolution. The platform was integrated into a double-barrel nanoprobe combining pH sensing with feedback-controlled distance dependance via Scanning Ion Conductance Microscopy. This allows for the simultaneous 3D topographical imaging and pHe monitoring of living cancer cells. These classes of nanoprobes were used for real-time high spatiotemporal resolution pHe mapping at the subcellular level and revealed tumour heterogeneity of the peri-cellular environments of melanoma and breast cancer cells.

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  40. Scanning Electrochemical Cell Microscopy for Analysis of Solid Electrolyte Interface on Negative Electrodes in Lithium-Ion Batteries

    Akichika Kumatani, Yuto Sato, Yasufumi Takahashi, Hitoshi Shiku, Tomokazu Matsue

    ECS Meeting Abstracts   Vol. {MA}2019-01 ( 47 ) page: 2267 - 2267   2019.5

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    <jats:p> Lithium-ion battery is one of the most popular secondary batteries for practical applications such as mobile phones and electrical cars because of their high energy density and good cyclability. For further improvement of their total performance with highly efficient cyclability, it is necessary to be in precise control of lithium-ion transport at the interface between electrolyte and electrodes. There is a major issue for efficient ion transport due to solid electrolyte interface (SEI) on negative composite electrodes such as graphite and/or silicon with some binders and electrical additives. The SEI is in general formed by decomposition of electrolyte. However, the SEI formation process or SEI itself is not still clear how the decomposition process proceeds due to the surface structure, binders or dispersion of active materials. Here, in this work we have used a scanning electrochemical microscopy (SECCM) with a single barrel nanopipette inside glove-box for analyzing local electrochemical reaction for SEI formation. A 50 nm radius nanopipette was filled with organic electrolyte (1.0 M LiPF<jats:sub>6</jats:sub> in ethylene carbonate:diethyl carbonate = 1:1 in vol. %) with a Li reference electrode. When the pipette was approached to the sample surface, a meniscus was created. Then, through the meniscus as a nanoscale electrochemical simulator, cyclic voltammogram was measured to introduce the SEI in localized area. The location SEI formed and their created potential were mapped by scanning the pipette on the sample. Further, on the particular structure such as basal and edge of graphite, the decomposition process was also analyzed for investigation of material structures for SEI formation. Those information would be particularly important to understand their mechanism and to control SEI formation. </jats:p>

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  41. Visualization of Inhomogeneuous Reactivity on Battery Material Using Scanning Electrochemical Cell Microscopy

    Takahashi Yasufumi, Inomata Hirotaka, Daiko Takamatsu, Akichika Kumatani, Hitoshi Shiku, Tomokazu Matsue

    ECS Meeting Abstracts   Vol. {MA}2019-01 ( 47 ) page: 2259 - 2259   2019.5

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    <jats:p> To understand the metal oxide coating effect on battery performance, the following two techniques are required: 1) constructing a flat thin-film electrode surface to realize a well-defined interface and 2) analyzing the electrode/electrolyte interface reaction with nanoscale resolution. We previously studied flat LiCoO<jats:sub>2</jats:sub> thin-film electrodes using<jats:italic> in situ</jats:italic> surface-sensitive X-ray absorption spectroscopy (XAS) and reported that Co reduction at the LiCoO<jats:sub>2</jats:sub> surface resulting from electrolyte contact caused the initial degradation. We also showed that the ZrO<jats:sub>2</jats:sub> layer successfully prevented physical contact between LiCoO<jats:sub>2</jats:sub> and the electrolyte. And it confirmed that a thicker ZrO<jats:sub>2</jats:sub> layer (above 2 nm) increased the diffusion resistance of the lithium ions in the ZrO<jats:sub>2</jats:sub> layer. However, since XAS lacks in-plane resolution and provides only averaged information, it is impossible to analyze the ZrO<jats:sub>2</jats:sub> morphology in detail. Recently, Taguchi et al. investigated a thin Li-Zr-layer (ca. 2 nm) on a LiCoO<jats:sub>2</jats:sub> composite electrode by transmission electron microscopy (TEM). They suggested that this thin layer could improve the durability.<jats:sup /> However, it is difficult to analyze the electrochemical properties using TEM. To evaluate the intrinsic mechanism of the metal oxide coating effect, it is necessary to develop a novel <jats:italic>in-situ</jats:italic> method that can analyze the surface morphology with high spatial resolution and simultaneously determine the local electrochemical properties. </jats:p>
    <jats:p>Scanning electrochemical microscopy (SECM) is a powerful technique for linking the surface morphology of a sample to its electrochemical properties. For the battery materials, the SECM feedback mode is effective in monitoring solid electrolyte interphase formation. To directly and quantitatively investigate spatially resolved ionic processes, mercury-capped platinum ultramicroelectrodes were developed and employed for Li<jats:sup>+</jats:sup> imaging based on Li stripping. However, it is difficult to visualize the Li<jats:sup>+</jats:sup> flux in battery materials at the sub-micrometer scale by SECM. Scanning electrochemical cell microscopy (SECCM), which uses a nanopipette as a probe and forms a local electrochemical cell, is effective in characterizing surface reactivity. We recently applied SECCM for visualization of electrochemical activities on a lithium-ion battery cathode material at sub-micrometer resolution. The SECCM was applied to collect or provide Li in specified area confined by the nanopipette. Further, it collection visualized the electrochemical properties by scanning the nanopipette as an image. There are some strong advantages in SECCM for battery material research such as its high spatial resolution, small capacitive current, and isolated electrochemical cell. </jats:p>
    <jats:p>In this report, we applied SECCM to characterize a ZrO<jats:sub>2</jats:sub>-coated LiCoO<jats:sub>2</jats:sub> thin-film electrode prepared by pulsed laser deposition. Local cyclic voltammetry (CV) and galvanostatic charge/discharge were performed to characterize the cycle durability and rate performance of ZrO<jats:sub>2</jats:sub>-coated LiCoO<jats:sub>2</jats:sub> thin-film electrodes and to reveal the relationship between the ZrO<jats:sub>2</jats:sub> morphology and thickness. </jats:p>

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  42. Nanoscale Electrochemical Cell Analysis for Formation of SEI on Negative Electrodes of Lithium-ion Batteries

    Kumatani Akichika, Sato Yuto, Takahashi Yasufumi, Shiku Hitoshi, Matsue Tomokazu

    JSAP Annual Meetings Extended Abstracts   Vol. 2019.1 ( 0 ) page: 1521 - 1521   2019.2

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  43. Nanoscale Electrochemical Imaging for Hydrogen Evolution Reaction on WS<sub>2</sub> mono-/bilayers

    Ogawa Hiroto, Kumatani Akichika, Endo Takahiko, Kobayashi Yu, Ida Hiroki, Takahashi Yasufumi, Matsue Tomokazu, Miyata Yasumitsu, Shiku Hitoshi

    JSAP Annual Meetings Extended Abstracts   Vol. 2019.1 ( 0 ) page: 3620 - 3620   2019.2

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    DOI: 10.11470/jsapmeeting.2019.1.0_3620

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  44. Scanning electrochemical cell microscopy for visualization and local electrochemical activities of lithium-ion (de) intercalation process in lithium-ion batteries electrodes

    Akichika Kumatani, Akichika Kumatani, Yasufumi Takahashi, Yasufumi Takahashi, Chiho Miura, Hiroki Ida, Hirotaka Inomata, Hitoshi Shiku, Hirokazu Munakata, Kiyoshi Kanamura, Tomokazu Matsue

    Surface and Interface Analysis   Vol. 51 ( 1 ) page: 27 - 30   2019.1

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    © 2018 John Wiley &amp; Sons, Ltd. Scanning electrochemical cell microscopy with a single barrel micro-/nano-pipette (SECCM) was applied to lithium iron phosphate (LiFePO4) composite positive electrodes and an isolated LiFePO4 secondary particle for lithium-ion batteries. To analyze lithium-ion (Li+) charge or discharge process on the electrodes using local probe, a pipette filled with LiCl electrolyte solution and Ag/AgCl quasi-reference counter electrode (QRCE) was used. Both the local electrochemical activities of LiFePO4 on the composite electrodes and a single particle were revealed by SECCM as in-situ direct measurement of current response-related Li+ transport from mapping and cyclic voltammogram at confined area by the pipette. The mapping has visualized Li+ deintercalation process from LiFePO4 at +0.65 V (applied between the sample-QRCE). We show that the SECCM system is a strong analytical tool for a characterization of local Li+ behavior of active electrode materials in lithium-ion batteries.

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  45. Chemical Dopants on Edge of Holey Graphene Accelerate Electrochemical Hydrogen Evolution Reaction

    Akichika Kumatani, Chiho Miura, Hirotaka Kuramochi, Tatsuhiko Ohto, Mitsuru Wakisaka, Yuki Nagata, Hiroki Ida, Yasufumi Takahashi, Kailong Hu, Samuel Jeong, Jun ichi Fujita, Tomokazu Matsue, Yoshikazu Ito

    Advanced Science   Vol. 6 ( 10 ) page: 1900119   2019.1

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    © 2019 The Authors. Published by WILEY-VCH Verlag GmbH &amp; Co. KGaA, Weinheim Carbon-based metal-free catalysts for the hydrogen evolution reaction (HER) are essential for the development of a sustainable hydrogen society. Identification of the active sites in heterogeneous catalysis is key for the rational design of low-cost and efficient catalysts. Here, by fabricating holey graphene with chemically dopants, the atomic-level mechanism for accelerating HER by chemical dopants is unveiled, through elemental mapping with atomistic characterizations, scanning electrochemical cell microscopy (SECCM), and density functional theory (DFT) calculations. It is found that the synergetic effects of two important factors—edge structure of graphene and nitrogen/phosphorous codoping—enhance HER activity. SECCM evidences that graphene edges with chemical dopants are electrochemically very active. Indeed, DFT calculation suggests that the pyridinic nitrogen atom could be the catalytically active sites. The HER activity is enhanced due to phosphorus dopants, because phosphorus dopants promote the charge accumulations on the catalytically active nitrogen atoms. These findings pave a path for engineering the edge structure of graphene in graphene-based catalysts.

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  46. Bioimaging by a Scanning Probe Microscope Using Microelectrodes and Nanopipettes

    Takahashi Yasufumi

    BUNSEKI KAGAKU   Vol. 68 ( 1 ) page: 33 - 41   2019.1

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  47. Bioimaging by a Scanning Probe Microscope Using Microelectrodes and Nanopipettes

    高橋康史

    分析化学   Vol. 68 ( 1 ) page: 33‐41(J‐STAGE) - 41   2019

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    <p>Scanning probe microscopy is an effective tool for nanoscale imaging and characterization at a solid-liquid interface. Scanning electrochemical microscopy (SECM) and the scanning ion conductance microscopy (SICM) using microelectrodes and nanopipettes as probes are applied to cell surface chemical and topographical imaging, respectively. In this review, we introduce our recent study concerning the development of nanoscale electrodes and a system for high-resolution of SECM, electrochemical imaging of membrane proteins, electrochemical evaluation of differentiation state of embryonic stem cells, hybrid system of SECM and SICM, neurotransmitters measurement, high-speed SICM, and chemical field effect transistor.</p>

    DOI: 10.2116/bunsekikagaku.68.33

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  48. In situ chemical sensing by using scanning probe microscope Reviewed

    Takahashi Yasufumi, Zhou Yuanshu, Fukuma Takeshi

    Folia Pharmacologica Japonica   Vol. 153 ( 6 ) page: 267 - 272   2019

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    &lt;p&gt;Scanning electrochemical microscopy (SECM), which utilizes microelectrodes as a probe to measure the chemicals released and consumed by cells as current signal, is a promising tool for measuring the metabolites of cells. We have improved SECM resolution for single cell imaging by miniaturizing the size of the electrode and developing hybrid system of SECM and scanning ion conductance microscopy (SICM), which utilizes nanopipette as a probe to measure live cell topography. SECM-SICM provides simultaneous imaging of concentration profiles of chemical substances and cell surface topography. Using this system, we successfully measured the release of neurotransmitters from PC12 cells. In addition, the nanoscale electrodes are useful for intracellular chemical detection by inserting the electrodes into cells and measured reactive oxygen species (ROS).&lt;/p&gt;

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  49. Visualization of primary cilia topography using scanning probe microscopy

    Takahashi Yasufumi, Zhou Yuanshu, Saito Masaki, Fukuma Takeshi

    Proceedings for Annual Meeting of The Japanese Pharmacological Society   Vol. 92 ( 0 ) page: 1-S09-3 - S09-3   2019

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    <p>Primary cilia are hair-like sensory organelles whose dimensions and location vary with cell type and culture condition. Herein, we employed scanning ion conductance microscopy (SICM) to visualize the topography of primary cilia from different cell types. By combining SICM with fluorescence imaging, we successfully distinguished between surface cilia that project outward from the cell surface and subsurface cilia that are trapped below it. The nanoscale structure of the ciliary pocket, which cannot be easily identified using a confocal fluorescence microscope, was observed in SICM images. Furthermore, we developed a topographic reconstruction method using current-distance profiles to evaluate the relationship between set point and topographic image and found that a low set point is important for detecting the true topography of a primary cilium using hopping mode SICM.</p>

    DOI: 10.1254/jpssuppl.92.0_1-s09-3

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  50. Nanoscale imaging of extracellular microenvironment using scanning ion conductance microscopy

    Takahashi Yasufumi, Zhou Yuanshu, Fujii Takuto, Sakai Hideki, Fukuma Takeshi

    Proceedings for Annual Meeting of The Japanese Pharmacological Society   Vol. 92 ( 0 ) page: 2-S14-3 - S14-3   2019

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    <p>Local metabolite and ionic strength are important factors for maintaining the functions of living cells. We have developed micro-nanoscale electrode and electrochemical sensor based scanning probe microscopy to measure the spatial electrochemical metabolite and ion concentration profile near the sample surface with nanoscale resolution. Scanning electrochemical microscopy (SECM) uses an ultramicroelectrode as a probe for detecting electroactive chemical species (oxygen, ATP, and reactive oxygen species (ROS), and neurotransmitter). SECM has been recognized as an effective tool for investigating micrometer-scale local chemical flux. Miniaturization of the electrode is an important factor for improving SECM resolution.<sup> </sup>Electrode–sample distance control is also an important factor for measuring fast chemical flux and improving SECM resolution. Distance control by ion current feedback is a promising way for the non-contact investigation of soft materials, SECM–scanning ion-conductance microscopy (SICM) has been used in a hybrid system to improve SECM resolution by controlling the electrode probe and sample distance in solutions without direct contact. SICM is also useful for detecting the ion concentration profile and charge measurement in a solution. We measured the 3D chemical and ion current using SECM–SICM. In this presentation, we report the SICM topography images of gastric surface mucous cell lines (GSM06), which produce periodic acid-schiff and concanavalin A positive glycoproteins. To visualize the damage process of the mucosal layer, we added ethanol to GSM06 cells and imaged the topography change using SICM. We also performed topography and electrochemical simultaneous imaging using SICM-SECM to identify the mucosal layer without labelling.</p>

    DOI: 10.1254/jpssuppl.92.0_2-s14-3

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  51. Unlabeled imaging of primary cilia by scanning ion conductance microscopy Reviewed

    Zhou Yuanshu, Saito Masaki, Fukuma Takeshi, Takahashi Yasufumi

    Folia Pharmacologica Japonica   Vol. 154 ( 4 ) page: 192 - 196   2019

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    &lt;p&gt;Primary cilia are non-motile cilia consisting of a centriole-derived basal body and a microtubule-based axoneme. In recent years, the structure and function of primary cilia have been attracting attention due to the relation with the onset of ciliary disease. Scanning ion conductance microscopy (SICM) is a probe microscopy used to measure the topography and functions of living cells at nanoscale. Furthermore, the labelling procedure is not necessary for SICM measurement compare to fluorescence imaging. We compared the structures of primary cilia of human retinal pigment epithelial cell line (RPE-1 cells) and Madin-Darby canine kidney cell line (MDCK cells) at nanoscale by using SICM. In addition, high resolution SICM images have also succeeded in visualizing ciliary pockets that difficult to be fluorescently labeled.&lt;/p&gt;

    DOI: 10.1254/fpj.154.192

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  52. 走査型プローブ顕微鏡 45.原子間力顕微鏡 ii.走査型イオンコンダクタンス顕微鏡―生細胞の形状と機能をナノスケールで可視化

    高橋康史

    実験医学   Vol. 36 ( 20 ) page: 3470‐3471   2018.12

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  53. Visualization of inhomogeneous current distribution on ZrO<sub>2</sub>-coated LiCoO<sub>2</sub> thin-film electrodes using scanning electrochemical cell microscopy. Reviewed

    Inomata H, Takahashi Y, Takamatsu D, Kumatani A, Ida H, Shiku H, Matsue T

    Chemical communications (Cambridge, England)   Vol. 55 ( 4 ) page: 545 - 548   2018.12

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    Cathode surface coating with metal-oxide thin layers has been intensively studied to improve the cycle durability of lithium-ion batteries. A comprehensive understanding of the metal-oxide morphology and the local electrochemical properties is essential for figuring out the metal-oxide coating effect. In this study, scanning electrochemical cell microscopy (SECCM) is used to analyze the surface morphology with high spatial resolution, together with the local electrochemical properties.

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  54. Quantitative Real-Time Monitoring of Antibody-Induced Internalization of Epidermal Growth Factor Receptor on Single Living Mammalian Cells Using Scanning Electrochemical Microscopy

    Yoshiharu Matsumae, Yoshiharu Matsumae, Yasufumi Takahashi, Yasufumi Takahashi, Yasufumi Takahashi, Yasufumi Takahashi, Hitoshi Shiku, Hitoshi Shiku, Tomokazu Matsue

    ChemElectroChem   Vol. 5 ( 20 ) page: 3096 - 3101   2018.10

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    © 2018 Wiley-VCH Verlag GmbH &amp; Co. KGaA, Weinheim An antibody-induced internalization of epidermal growth factor receptor (EGFR) was quantitatively monitored using scanning electrochemical microscopy (SECM) at the single-cell level. The antibody Cetuximab is used for cancer treatment because of its capability to bind and internalize EGFR, which is one of the key membrane proteins associated with many cancers. To monitor antibody-induced EGFR internalization, Cetuximab was simply labelled with enzymes and the resulting enzymatic products were then electrochemically detected by using a microelectrode. By optimizing experimental parameters, such as immunostaining condition, enzyme type, and buffer solution, we were able to successfully monitor the EGFR internalization by using SECM, from which we found a decrease in current responses from a single living cell by 20 % in the first 60 min, suggesting different internalization pathways from inherent ligand-induced internalization.

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  55. 超解像度ケミカルイメージングを実現する電気化学顕微鏡の開発

    高橋康史

    バイオサイエンスとインダストリー   Vol. 76 ( 4 ) page: 332‐333   2018.7

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  56. ナノ電気化学顕微鏡の創成と単一細胞評価への応用

    高橋康史

    中谷医工計測技術振興財団年報   ( 31 ) page: 109‐114   2018.3

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  57. 酸化還元反応の差異による半導体・金属カーボンナノチューブの検出

    熊谷明哉, 熊谷明哉, 志村実優, 高橋康史, 高橋康史, 三浦千穂, 岡田健, 岡田健, 井田大貴, 珠玖仁, 寒川誠二, 寒川誠二, 末永智一

    応用物理学会春季学術講演会講演予稿集(CD-ROM)   Vol. 65th   page: ROMBUNNO.17p‐P5‐4   2018.3

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  58. 電気化学イメージングによる金属/半導体カーボンナノチューブの酸化還元反応の検証

    志村実優, 熊谷明哉, 熊谷明哉, 岡田健, 三浦千穂, 井田大貴, 寒川誠二, 寒川誠二, 珠玖仁, 高橋康史, 高橋康史, 末永智一

    電気化学会大会講演要旨集(CD-ROM)   Vol. 85th   page: ROMBUNNO.1J12   2018.2

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  59. Nanoscale Imaging of Primary Cilia with Scanning Ion Conductance Microscopy Reviewed

    Yuanshu Zhou, Masaki Saito, Takafumi Miyamoto, Pavel Novak, Andrew I Shevchuk, Yuri E Korchev, Takeshi Fukuma, Yasufumi Takahashi

    Analytical Chemistry   Vol. 90 ( 4 ) page: 2891 - 2895   2018.2

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    Primary cilia are hair-like sensory organelles whose dimensions and location vary with cell type and culture condition. Herein, we employed scanning ion conductance microscopy (SICM) to visualize the topography of primary cilia from different cell types. By combining SICM with fluorescence imaging, we successfully distinguished between surface cilia that project outward from the cell surface and subsurface cilia that are trapped below it. The nanoscale structure of the ciliary pocket, which cannot be easily identified using a confocal fluorescence microscope, was observed in SICM images. Furthermore, we developed a topographic reconstruction method using current-distance profiles to evaluate the relationship between set point and topographic image and found that a low set point is important for detecting the true topography of a primary cilium using hopping mode SICM.

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  60. Erratum to: An approach to the research on ion and water properties in the interphase between the plasma membrane and bulk extracellular solution. Reviewed

    Hiroshi Hibino, Madoka Takai, Hidenori Noguchi, Seishiro Sawamura, Yasufumi Takahashi, Hideki Sakai, Hitoshi Shiku

    The journal of physiological sciences : JPS   Vol. 68 ( 1 ) page: 101 - 101   2018.1

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    The article An approach to the research on ion and water properties in the interphase between the plasma membrane and bulk extracellular solution, written by Hiroshi Hibino, Madoka Takai, Hidenori Noguchi, Seishiro Sawamura, Yasufumi Takahashi, Hideki Sakai and Hitoshi Shiku, was originally published Online First without open access.

    DOI: 10.1007/s12576-017-0572-6

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  61. Super-resolution chemical imaging for live cell using scanning probe microscopy

    Takahashi Yasufumi

    Meeting Abstracts of the Physical Society of Japan   Vol. 73.1 ( 0 ) page: 3049 - 3049   2018

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    DOI: 10.11316/jpsgaiyo.73.1.0_3049

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  62. 細胞多様性解明に資する光技術―見て,動かす I.見る,観る,視る 走査型プローブ顕微鏡よる生細胞の超解像イメージング

    高橋康史

    生体の科学   Vol. 68 ( 5 ) page: 382‐383 - 383   2017.10

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  63. Development of carbon-based nanoelectrodes for biosensing and electrochemical imaging Reviewed

    Yasufumi Takahashi, Yuanshu Zhou, Takeshi Fukuma

    Current Opinion in Electrochemistry   Vol. 5 ( 1 ) page: 121 - 125   2017.10

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    Carbon nanoelectrodes are emerging as a powerful tool for local electrochemical measurements. In addition to the advantages of carbon electrodes, i.e., their electrochemical catalytic property, high current density, low ohmic drop, low capacitive current, wide potential window, and minimal electrode fouling, nanoscale spatial resolution opens up new possibilities for single synapse and intracellular measurements as well as for high sensitive chemical measurements. In this review, we present the recent progress made in the applications of carbon nanoelectrodes, mainly in electrochemical sensing and electrochemical imaging.

    DOI: 10.1016/j.coelec.2017.07.014

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  64. 3D electrochemical and ion current imaging using scanning electrochemical-scanning ion conductance microscopy Reviewed

    Yasufumi Takahashi, Hiroki Ida, Yoshiharu Matsumae, Hirokazu Komaki, Yuanshu Zhou, Akichika Kumatani, Makoto Kanzaki, Hitoshi Shiku, Tomokazu Matsue

    PHYSICAL CHEMISTRY CHEMICAL PHYSICS   Vol. 19 ( 39 ) page: 26728 - 26733   2017.10

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    Local cell-membrane permeability and ionic strength are important factors for maintaining the functions of cells. Here, we measured the spatial electrochemical and ion concentration profile near the sample surface with nanoscale resolution using scanning electrochemical microscopy (SECM) combined with scanning ion-conductance microscopy (SICM). The ion current feedback system is an effective way to control probe-sample distance without contact and monitor the kinetic effect of mediator regeneration and the chemical concentration profile. For demonstrating 3D electrochemical and ion concentration mapping, we evaluated the reaction rate of electrochemical mediator regeneration on an unbiased conductor and visualized inhomogeneous permeability and the ion concentration 3D profile on a single fixed adipocyte cell surface.

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  65. An approach to the research on ion and water properties in the interphase between the plasma membrane and bulk extracellular solution Reviewed

    Hiroshi Hibino, Madoka Takai, Hidenori Noguchi, Seishiro Sawamura, Yasufumi Takahashi, Hideki Sakai, Hitoshi Shiku

    JOURNAL OF PHYSIOLOGICAL SCIENCES   Vol. 67 ( 4 ) page: 439 - 445   2017.7

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    In vivo, cells are immersed in an extracellular solution that contains a variety of bioactive substances including ions and water. Classical electrophysiological analyses of epithelial cells in the stomach and small intestine have revealed that within a distance of several hundred micrometers above their apical plasma membrane, lies an extracellular layer that shows ion concentration gradients undetectable in the bulk phase. This "unstirred layer", which contains stagnant solutes, may also exist between the bulk extracellular solution and membranes of other cells in an organism and may show different properties. On the other hand, an earlier study using a bacterial planar membrane indicated that H+ released from a transporter migrates in the horizontal direction along the membrane surface much faster than it diffuses vertically toward the extracellular space. This result implies that between the membrane surface and unstirred layer, there is a "nanointerface" that has unique ionic dynamics. Advanced technologies have revealed that the nanointerface on artificial membranes possibly harbors a highly ordered assembly of water molecules. In general, hydrogen bonds are involved in formation of the ordered water structure and can mediate rapid transfer of H+ between neighboring molecules. This description may match the phenomenon on the bacterial membrane. A recent study has suggested that water molecules in the nanointerface regulate the gating of K+ channels. Here, the region comprising the unstirred layer and nanointerface is defined as the interphase between the plasma membrane and bulk extracellular solution (iMES). This article briefly describes the physicochemical properties of ions and water in the iMES and their physiological significance. We also describe the methodologies that are currently used or will be applicable to the interphase research.

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  66. High Speed Scanning Ion Conductance Microscopy for Quantitative Analysis of Nanoscale Dynamics of Microvilli Reviewed

    Hiroki Ida, Yasufumi Takahashi, Akichika Kumatani, Hitoshi Shiku, Tomokazu Matsue

    ANALYTICAL CHEMISTRY   Vol. 89 ( 11 ) page: 6016 - 6021   2017.6

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    Observation of nanoscale structure dynamics on cell surfaces is essential-to understanding cell functions. Hopping Mode, scanning ion conductance microscopy (SICM) was used to visualize the topography, of fragile convoluted nanoscale structures on cell surfaces under noninvasive conditions. However, conventional hopping mode SICM does not have sufficient temporal resolution to observe cell-surface dynamics in situ because of the additional time required for performing vertical probe movements of the nanopipette. Here, we introduce a new scanning algorithm for high speed SICM measurements using low capacitance and high-resonance-frequency piezo stages. As a result, a topographic image is taken within 18 s with a 64 x 64 pixel resolution at 10 X 10 mu m. The high speed SICM is applied to the characterization of microvilli dynamics on surfaces, which shows clear structural changes after the epidermal growth factor stimulation.

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  67. Loosening of Lipid Packing Promotes Oligoarginine Entry into Cells Reviewed

    Tomo Murayama, Toshihiro Masuda, Sergii Afonin, Kenichi Kawano, Tomoka Takatani-Nakase, Hiroki Ida, Yasufumi Takahashi, Takeshi Fukuma, Anne S. Ulrich, Shiroh Futaki

    ANGEWANDTE CHEMIE-INTERNATIONAL EDITION   Vol. 56 ( 26 ) page: 7644 - 7647   2017.6

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    Despite extensive use of arginine-rich cell-penetrating peptides (CPPs)-including octaarginine (R8)-as intracellular delivery vectors, mechanisms for their internalization are still under debate. Lipid packing in live cell membranes was characterized using a polarity-sensitive dye (di-4-ANEPPDHQ), and evaluated in terms of generalized polarization. Treatment with membrane curvature-inducing peptides led to significant loosening of the lipid packing, resulting in an enhanced R8 penetration. Pyrenebutyrate (PyB) is known to facilitate R8 membrane translocation by working as a hydrophobic counteranion. Interestingly, PyB also actively induced membrane curvature and perturbed lipid packing. R8 is known to directly cross cell membranes at elevated concentrations. The sites of R8 influx were found to have looser lipid packing than surrounding areas. Lipid packing loosening is proposed as a key factor that governs the membrane translocation of CPPs.

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  68. Advanced Scanning Electrochemical Microscope System for High-Resolution imaging and Electrochemical Applications

    Ryo Matsuoka, Shigeo Aoyagi, Naoshi Matsumoto, Masaaki Matsudaira, Yasufumi Takahashih, Akichika Kumatanid, Hiroki Ida, Hirokazu Munakata, Katsuhiko Iida, Hitoshi Shiku, Kiyoshi Kanamura, Tomokazu Matsue

    ELECTROCHEMISTRY   Vol. 85 ( 6 ) page: 319 - 326   2017.6

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    We developed three modes of high resolution scanning probe microscope system based on electrochemical principles, scanning ion conductance microscopy (SICM), scanning electrochemical microscopy-scanning ion conductance microscopy (SECM-SICM), and scanning electrochemical cell microscopy (SECCM). Firstly, a developed SICM system was constructed with a nanopipette filled with electrolyte solution as a probe. High resolution topographic images of NanoCulture (R) Plate with hexagonal chambers with 2 mu m-width banks, electro-deposited PEDOT (poly(3,4-ethylenedioxythiophane)) film, and fixed human squamous cell carcinoma were captured by the SICM. Second, SECM-SICM was performed with a double-barrel carbon nanoprobe. The one barrel of the nanoprobe was filled with carbon and used for SECM apparatus, the other barrel was filled with electrolyte for SICM configurations. Using the SECM-SICM system, simultaneous topographic and electrochemical images of micro-band electrodes with 10 pm-width line and space, and a cathode site of corrosion in the aluminum die gusto with submicron spatial resolution were obtained. Thirdly, the SECCM featuring a nanopipette probe filled with LiCI electrolyte was applied for obtaining topographies and images of current activity of a LiFePO4 electrode. (C) The Electrochemical Society of Japan, All rights reserved.

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  69. Continuous collection and simultaneous detection of picoliter volume of nucleic acid samples using a mille-feuille probe Reviewed

    Hidenori Ito, Motoki Tanaka, Yuanshu Zhou, Yuji Nashimoto, Yasufumi Takahashi, Kosuke Ino, Tomokazu Matsue, Hitoshi Shiku

    ANALYTICAL AND BIOANALYTICAL CHEMISTRY   Vol. 409 ( 4 ) page: 961 - 969   2017.2

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    Investigation of the positional heterogeneity of messenger RNA (mRNA) expression in tissues requires a technology that facilitates analysis of mRNA expression in the selected single cells. We developed a mille-feuille probe (MP) that allows the lamination of the aqueous and organic phases in a nanopipette under voltage control. The MP was used for continuous collection of different nucleic acid samples and sequential evaluation of gene expression with mRNA barcoding tags. First, we found that the aqueous phases could be laminated into five individual layers and separated by the plugs of the organic phases in a nanopipette when the salt (THATPBCl) concentration in the organic phase was 100 mM. Second, the aspiration rate of the MP was stabilized and the velocity of the aqueous phase in the MP was lowered at higher THATPBCl concentrations in the organic phase. This was because the force during ingression of the aqueous phase into the organic - phase-filled nanopipette induced an electro-osmotic flow between the inside wall of the nanopipette and THATPBCl in the organic phase. Third, inclusion of mRNA barcoding tags in the MP facilitated complementary DNA construction and sequential analysis of gene expression. This technique has potential to be applicable to RNA sequencing from different cell samples across the life sciences.

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  70. Scanning Probe Microscopy for Nanoscale Electrochemical Imaging Reviewed

    Yasufumi Takahashi, Akichika Kumatani, Hitoshi Shiku, Tomokazu Matsue

    ANALYTICAL CHEMISTRY   Vol. 89 ( 1 ) page: 342 - 357   2017.1

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    DOI: 10.1021/acs.analchem.6b04355

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  71. Development of interface ion conductance microscopy for visualising nanoscale ion transfer pass

    高橋康史

    旭硝子財団助成成果報告書(Web)   Vol. 2017   page: ROMBUNNO.11 (WEB ONLY) - 7   2017

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  72. Cell sheet fabrication using RGD peptide-coupled alginate hydrogels fabricated by an electrodeposition method Reviewed

    Fumisato Ozawa, Kosuke Ino, Hitoshi Shiku, Tomokazu Matsue

    Chemistry Letters   Vol. 46 ( 4 ) page: 605 - 608   2017

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    A novel and simple method for constructing cell sheets is described in which culture surfaces were modified with RGD peptide-coupled alginate hydrogels using an electrodeposition method. Cells were cultured on the hydrogels to form a contiguous cell sheet-like structure. Then, the hydrogels were dissolved by addition of an EDTA solution and the cell sheets rapidly detached from the surface. This is the first report of the fabrication of cell sheets on RGD peptide-coupled alginate hydrogels using an electrodeposition method. We believe the technique is useful for cell sheet engineering.

    DOI: 10.1246/cl.170003

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  73. 高解像度走査型電気化学顕微鏡の開発 Reviewed

    高橋康史

    化学と工業   Vol. 69 ( 9 ) page: 777 - 779   2016.9

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  74. Development of High-Resolution Scanning Electrochemical Microscopy for Nanoscale Topography and Electrochemical Simultaneous Imaging Reviewed

    Yasufumi Takahashi

    ELECTROCHEMISTRY   Vol. 84 ( 9 ) page: 662 - 666   2016.9

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    This article reviews our recent progress in the development of high-resolution scanning electrochemical microscopy (SECM) and its application to biological samples. SECM uses an ultramicroelectrode (UME) as a probe and a scanning mechanical stage for controlling the probe position. To improve the resolution of SECM, we have developed a fabrication method for pyrolytic carbon nanoelectrodes and a current feedback system for probe sample distance control. The current feedback system effectively provides high-quality electrochemical and non contact topography images because the current signal depends on the probe-sample distance. High-resolution SECM has overcome the limit of microscale imaging resolution and enabled the imaging of local regions within cells. In this study, we address four topics: nanoelectrode fabrication, current feedback probe-sample distance control systems, membrane protein imaging, and neurotransmitter detection. (C) The Electrochemical Society of Japan, All rights reserved.

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  75. Evaluation of mRNA Localization Using Double Barrel Scanning Ion Conductance Microscopy Reviewed

    Yuji Nashimoto, Yasufumi Takahashi, Yuanshu Zhou, Hidenori Ito, Hiroki Ida, Kosuke Ino, Tomokazu Matsue, Hitoshi Shiku

    ACS Nano   Vol. 10 ( 7 ) page: 6915 - 6922   2016.7

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    Information regarding spatial mRNA localization in single cells is necessary for a better understanding of cellular functions in tissues. Here, we report a method for evaluating localization of mRNA in single cells using double barrel scanning ion conductance microscopy (SICM). Two barrels in a nanopipette were filled with aqueous and organic electrolyte solutions and used for SICM and as an electrochemical syringe, respectively. We confirmed that the organic phase barrel could be used to collect cytosol from living cells, which is a minute but sufficient amount to assess cellular status using qPCR analysis. The water phase barrel could be used for SICM to image topography with subcellular resolution, which could be used to determine positions for analyzing mRNA expression. This system was able to evaluate mRNA localization in single cells. After puncturing the cellular membrane in a minimally invasive manner, using SICM imaging as a guide, we collected a small amount cytosol from different positions within a single cell and showed that mRNA expression depends on cellular position. In this study, we show that SICM imaging can be utilized for the analysis of mRNA localization in single cells. In addition, we fully automated the pipet movement in the XYZ-directions during the puncturing processes, making it applicable as a high-throughput system for collecting cytosol and analyzing mRNA localization.

    DOI: 10.1021/acsnano.6b02753

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  76. Liquid-junction-free system for substitutional stripping voltammetry using a closed bipolar electrode system Reviewed

    Shinichiro Takano, Kumi Y. Inoue, Miho Ikegawa, Yasufumi Takahashi, Kosuke Ino, Hitoshi Shiku, Tomokazu Matsue

    ELECTROCHEMISTRY COMMUNICATIONS   Vol. 66   page: 34 - 37   2016.5

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    A liquid-junction-free electrochemical system has been developed for substitutional stripping voltammetry (SSV). SSV is a type of stripping analysis that changes the redox current to metal deposition. Generally, SSV requires a liquid junction to maintain electrical conductivity between separated cells. In this report, a closed bipolar electrode system(cBPES) was used to perform SSV without a liquid junction. In this system, electrical conductivity between separated cells was maintained using driving electrodes inserted into each cell. We demonstrated quantification of p-aminophenol (pAP) using a liquid-junction-free system for SSV. We investigated the effect of electrode area ratio on the BPE and the concentration ratio of redox species present in each cell. Then, we calibrated the pAP. A linear relationship between pAP concentration and SSV electrical charge was successfully obtained using our liquid-junction-free system, based on cBPES. This novel analytical system is a promising method for the fabrication of a compact SSV sensor for highly sensitive detections. (C) 2016 Elsevier B.V. All rights reserved.

    DOI: 10.1016/j.elecom.2016.02.014

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  77. Redox Cycling-based Electrochemical Reporter Gene Assay for Single Cells Using a Scanning Electrochemical Microscope-microwell System

    Hiroki Ida, Kosuke Ino, Junya Suzuki, Yasufumi Takahashi, Hitoshi Shiku, Tomokazu Matsue

    ELECTROCHEMISTRY   Vol. 84 ( 5 ) page: 308 - 311   2016.5

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    Single-cell analyses are important for providing new insights into cellular biology. Here we report an electrochemical reporter gene assay for single cells using a scanning electrochemical microscope (SECM)-microwell system. Each microwell trapped a single cell that synthesized a reporter protein, secreted alkaline phosphatase (SEAP). The SEAP catalyzed the hydrolysis of p-aminophenyl phosphate to p-aminophenol (PAP). A disk electrode in the SECM was positioned above the microwell and monitored the oxidation currents of PAP derived from SEAP. In addition, ring electrodes were prepared on the microwell device to induce redox cycling between the ring and disk electrodes, thus amplifying the electrochemical signals from the reporter protein. The redox cycling-based electrochemical reporter gene assay is useful for single-cell analyses. (C) The Electrochemical Society of Japan, All rights reserved.

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  78. Spearhead Nanometric Field-Effect Transistor Sensors for Single-Cell Analysis Reviewed

    Yanjun Zhang, Jan Clausmeyer, Babak Babakinejad, Ainara Lopez Cordoba, Tayyibah Ali, Andrew Shevchuk, Yasufumi Takahashi, Pavel Novak, Christopher Edwards, Max Lab, Sahana Gopal, Ciro Chiappini, Uma Anand, Luca Magnani, R. Charles Coombes, Julia Gorelik, Tomokazu Matsue, Wolfgang Schuhmann, David Klenerman, Elena V. Sviderskaya, Yuri Korchev

    ACS NANO   Vol. 10 ( 3 ) page: 3214 - 3221   2016.3

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    Nanometric field-effect-transistor (FET) sensors are made on the tip of spear-shaped dual carbon nanoelectrodes derived from carbon deposition inside double-barrel nanopipettes. The easy fabrication route allows deposition of semiconductors or conducting polymers to comprise the transistor channel. A channel from electrodeposited poly pyrrole (PPy) exhibits high sensitivity toward pH changes. This property is exploited by immobilizing hexokinase on PPy nano-FETs to give rise to a selective ATP biosensor. Extracellular pH and ATP gradients are key biochemical constituents in the microenvironment of living cells; we monitor their real-time changes in relation to cancer cells and cardiomyocytes. The highly localized detection is possible because of the high aspect ratio and the spear-like design of the nano-FET probes. The accurately positioned nano-FET sensors can detect concentration gradients in three-dimensional space, identify biochemical properties of a single living cell, and after cell membrane penetration perform intracellular measurements.

    DOI: 10.1021/acsnano.5b05211

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  79. Chemical concentration profile imaging using scanning electrochemical microscopy and scanning ion conductance microscopy hybrid system

    Takahashi Yasufumi, Ida Hiroki, Zhou Yuanshu, Shiku Hitoshi, Matsue Tomokazu

    JOURNAL OF PHARMACOLOGICAL SCIENCES   Vol. 130 ( 3 ) page: S32 - S32   2016.3

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  80. Localized Gene Expression Analysis during Sprouting Angiogenesis in Mouse Embryoid Bodies Using a Double Barrel Carbon Probe Reviewed

    Hidenori Ito, Yuji Nashimoto, Yuanshu Zhou, Yasufumi Takahashi, Kosuke Ino, Hitoshi Shiku, Tomokazu Matsue

    ANALYTICAL CHEMISTRY   Vol. 88 ( 1 ) page: 610 - 613   2016.1

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    The mouse embryonic stem (ES) cell-derived angiogenesis model is widely used as a 3D model, reproducing cell cell interactions in the living body. Previously, many methods to analyze localized cellular function, including in situ hybridization and laser capture microdissection, have been reported. In this study, we achieved a collection of localized cells from the angiogenesis model in hydrogel. The gene expression profiles of the endothelial cells derived from mouse ES cells were evaluated. First, we collected localized cells from the live tissue model embedded in hydrogel using the double barrel carbon probe (DBCP) and quantified mRNA expression. Second, we found that vascular marker genes were expressed at a much higher level in sprouting vessels than in the central core of the embryoid body because the cells in sprouting vessels might significantly differentiate into endothelial linages, including tip/stalk cells. Third, the gene expression levels tended to be different between the top and middle regions in the sprouting vessel due to the difference in the degree of differentiation in these regions. At the top region of the vessel, both the tip and stalk cells were present. The cells in the middle region became more mature. Collectively, these results show that DBCP is very useful for analyzing localized gene expression in cells collected from 3D live tissues embedded in hydrogel. This technique can be applied to comprehensive gene expression analyses in the medical field.

    DOI: 10.1021/acs.analchem.5b04338

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  81. Development of Nano Electrochemical Microscopy for Visualizing Nanoscale Cell Surface Topography and Chemical Profile

    TAKAHASHI Yasufumi

    Seibutsu Butsuri   Vol. 56 ( 3 ) page: 179 - 180   2016

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    DOI: 10.2142/biophys.56.179

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  82. Localized Electrochemical Analyses on Electrodes Using by Nano-Scanning Electrochemical Cell Microscopy

    KUMATANI Akichika, TAKAHASHI Yasufumi, MIURA Chiho, WATANABE Tetsuya, INOMATA Hirotaka, MUNAKATA Hirokazu, SHIKU Hitoshi, KANAMURA Kiyoshi, MATSUE Tomokazu

    Hyomen Kagaku   Vol. 37 ( 10 ) page: 494 - 498   2016

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    &lt;p&gt;Scanning electrochemical cell microscopy with a single barrel nanopipette (nanoSECCM), which is one of scanning electrochemical microscope (SECM) families, is a powerful tool for analyzing electrochemical activities (e.g. redox reaction and lithium-ion (de) intercalation processes) at localized area. A glass nano-pipette is used as a probe of nanoSECCM filled with electrolyte and a reference electrode. As the pipette is in proximity of sample surface, a meniscus is created. Through the meniscus, electrochemical activities can be obtained at localized area on the sample. Further, as the pipette scans the sample surface, electrochemical activities can be also visualized. Our experiments demonstrate that nanoSECCM is applicable to investigation of current response related to lithium-ion transport, redox cycling on various types of electrodes.&lt;/p&gt;

    DOI: 10.1380/jsssj.37.494

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  83. Electrochemical Imaging of Dopamine Release from Three-Dimensional-Cultured PC12 Cells Using Large-Scale Integration-Based Amperometric Sensors Reviewed

    Hiroya Abe, Kosuke Ino, Chen-Zhong Li, Yusuke Kanno, Kumi Y. Inoue, Atsushi Suda, Ryota Kunikata, Masahki Matsudaira, Yasufumi Takahashi, Hitoshi Shiku, Tomokazu Matsue

    ANALYTICAL CHEMISTRY   Vol. 87 ( 12 ) page: 6364 - 6370   2015.6

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    In the present study, we used a large-scale integration (LSI)-based amperometric sensor array system, designated Bio-LSI, to image dopamine release from three-dimensional (3D)-cultured PC12 cells (PC12 spheroids). The Bio-LSI device consists of 400 sensor electrodes with a pitch of 250 mu m for rapid electroehemical imaging of large, areas. PC12 spheroids were stimulated with K+ to release dopamine. Poststimulation dopai-nine release fibril the PC12 spheroids was electrochemically imaged using the Bio-LSI device. Bia-LSI clearly showed the effects of the dopaminergic drugs L-3,4-dihydroxyphenylalanine (L-DOPA) and reserpine on K+-stimulated dopamine release from PC12 spheroids. Out results demonstrate that dopamine release from PC12 spheroids can be monitored using the device, suggesting that the Bio-LSI is a promising tool for use in evaluating 3D-cultured dopaminergic cells and the effects of dopaminergic drugs. To the best of our knowledge, this report is the first to describe electrochemical imaging of dopamine release by PC12 spheroids using LSI-based amperometric sensors.

    DOI: 10.1021/acs.analchem.5b01307

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  84. エネルギーデバイスの最前線 電気化学セル顕微鏡を用いた電池材料表面における充放電特性のナノスケール画像化技術 Reviewed

    高橋康史, 熊谷明哉, 猪又宏貴, 珠玖仁, 末永智一

    エネルギーデバイス   Vol. 2 ( 4 ) page: 66 - 69   2015.4

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  85. Improving the Electrochemical Imaging Sensitivity of Scanning Electrochemical Microscopy-Scanning Ion Conductance Microscopy by Using Electrochemical Pt Deposition Reviewed

    Mustafa Sen, Yasufumi Takahashi, Yoshiharu Matsumae, Yoshiko Horiguchi, Akichika Kumatani, Kosuke Ino, Hitoshi Shiku, Tomokazu Matsue

    ANALYTICAL CHEMISTRY   Vol. 87 ( 6 ) page: 3484 - 3489   2015.3

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    We fabricated a platinum-based double barrel probe for scanning electrochemical microscopy scanning ion conductance microscopy (SECM-SICM) by electrodepositing platinum onto the carbon nanoelectrode of the double barrel probe. The deposition conditions were optimized to attain highly sensitive electrochemical measurements and imaging. Simultaneous SECM-SICM imaging of electrochemical features and noncontact topography by using the optimized probe afforded high-resolution images of epidermal growth factor receptors (EGFR) on the membrane surface of the A431 cells.

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  86. Nanoscale Imaging of an Unlabeled Secretory Protein in Living Cells Using Scanning Ion Conductance Microscopy Reviewed

    Yuji Nashimoto, Yasufumi Takahashi, Hiroki Ida, Yoshiharu Matsumae, Kosuke Ino, Hitoshi Shiku, Tomokazu Matsue

    ANALYTICAL CHEMISTRY   Vol. 87 ( 5 ) page: 2542 - 2545   2015.3

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    Scanning ion conductance microscopy (SICM) was applied to evaluate an unlabeled secretory protein in living cells. The target protein, von Willebrand factor (vWF), was released from human endothelial cells by adding phorbol-12-myristate-13-acetate (PMA). We confirmed that SICM could be used to clearly visualize the complex network of vWF and to detect strings with widths as low as 60 nm without any artifact. By acquiring the sequential SICM images of living cells, the protrusion and strings formation were observed. We also detected the opening and closing motions of a small pore (similar to 500 nm), which is difficult to visualize with fluorescence methods. The results clearly demonstrate that SICM is a powerful tool to examine the changes in living cells during exocytosis.

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  87. Scanning electrochemical microscopy for imaging single cells and biomolecules Reviewed

    Yasufumi Takahashi, Hitoshi Shiku, Tomokazu Matsue

    Nanobiosensors and Nanobioanalyses     page: 335 - 352   2015.1

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    This article presents an overview of the recent progress in scanning electrochemical microscopy (SECM) for imaging single cells and biomolecules. SECM is a technique for characterizing the local electrochemical nature of various materials by scanning a probe microelectrode. The probe current reflects the electrochemical processes occurring in the small space surrounded by the probe and the substrate. The spatial resolution of SECM is inferior to conventional scanning probe microscopes such as scanning tunneling microscopy (STM) and atomic force microscopy (AFM), since the fabrication of the probe microelectrodes with nanometer sizes is quite difficult. However, recent progress in the fabrication of nanometer-scale electrodes and the development of electrode-sample distance control systems has greatly enhanced the capacity of SECM systems to solve problems in cell biology. The topics reviewed include the following: enzyme activity evaluation, electrochemical enzyme-linked immunosorbent assays, membrane permeability evaluation, respiratory activity measurements, reporter gene assays, membrane protein imaging, and neurotransmitter detection.

    DOI: 10.1007/978-4-431-55190-4_16

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  88. Lsi-based amperometric device for electrochemical imaging of drug effect on dopamine release from three-dimensional cultured pc12 cells Reviewed

    H. Abe, K. Ino, C. Z. Li, Y. Kanno, K. Y. Inoue, A. Suda, R. Kunikata, M. Matsudaira, Y. Takahashi, H. Shiku, T. Matsue

    MicroTAS 2015 - 19th International Conference on Miniaturized Systems for Chemistry and Life Sciences     page: 1598 - 1600   2015

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    © 15CBMS-0001. We report a large-scale integration (LSI) based amperometric chip device containing 400 sensors with a pitch of 250 μm and its applications for biological analysis of dopamine release from three-dimensional (3D) cultured cells using rat pheochromocytoma (PC12) cells as a neural cell model. The 3D cultured PC12 cells (PC12 spheroids) were stimulated with a high K+ solution to induce dopamine release. We showed clearly drug effects of dopaminergic drugs L-3,4-dihydroxyphenylalanine, (L-DOPA) and reserpine on dopamine release from PC12 spheroids. Our results indicate that the device is a useful tool for evaluating the effects of dopaminergic drugs.

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  89. Nano-Scale Topography Imaging of Live Cell Surface Using Scanning Ion Conductance Microscopy Reviewed

    井田大貴, 高橋康史, 高橋康史, 高橋康史, 珠玖仁, 末永智一, 末永智一

    表面科学   Vol. 36 ( 6 ) page: 313-318 (J-STAGE)   2015

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    DOI: 10.1380/jsssj.36.313

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  90. Nanoscale visualization of redox activity at lithium-ion battery cathodes Reviewed

    Yasufumi Takahashi, Akichika Kumatani, Hirokazu Munakata, Hirotaka Inomata, Komachi Ito, Kosuke Ino, Hitoshi Shiku, Patrick R. Unwin, Yuri E. Korchev, Kiyoshi Kanamura, Tomokazu Matsue

    NATURE COMMUNICATIONS   Vol. 5   page: 5450   2014.11

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    Intercalation and deintercalation of lithium ions at electrode surfaces are central to the operation of lithium-ion batteries. Yet, on the most important composite cathode surfaces, this is a rather complex process involving spatially heterogeneous reactions that have proved difficult to resolve with existing techniques. Here we report a scanning electrochemical cell microscope based approach to define a mobile electrochemical cell that is used to quantitatively visualize electrochemical phenomena at the battery cathode material LiFePO4, with resolution of similar to 100 nm. The technique measures electrode topography and different electrochemical properties simultaneously, and the information can be combined with complementary microscopic techniques to reveal new perspectives on structure and activity. These electrodes exhibit highly spatially heterogeneous electrochemistry at the nanoscale, both within secondary particles and at individual primary nanoparticles, which is highly dependent on the local structure and composition.

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  91. Electrochemical monitoring of intracellular enzyme activity of single living mammalian cells by using a double-mediator system Reviewed

    Yoshiharu Matsumae, Yasufumi Takahashi, Kosuke Ino, Hitoshi Shiku, Tomokazu Matsue

    ANALYTICA CHIMICA ACTA   Vol. 842   page: 20 - 26   2014.9

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    We evaluated the intracellular NAD(P) H:quinone oxidoreductase (NQO) activity of single HeLa cells by using the menadione-ferrocyanide double-mediator system combined with scanning electrochemical microscopy (SECM). The double-mediator system was used to amplify the current response from the intracellular NQO activity and to reduce menadione-induced cell damage. The electron shuttle between the electrode and menadione was mediated by the ferrocyanide/ferricyanide redox couple. Generation of ferrocyanide was observed immediately after the addition of a lower concentration (10 mu M) of menadione. The ferrocyanide generation rate was constant for 120 min. At a higher menadione concentration (100 mu M), the ferrocyanide generation rate decreased within 30 min because of the cytotoxic effect of menadione. We also investigated the relationship between intracellular reactive oxygen species or glutathione levels and exposure to different menadione concentrations to determine the optimal condition for SECM with minimal invasiveness. The present study clearly demonstrates that SECM is useful for the analysis of intracellular enzymatic activities in single cells with a double-mediator system. (C) 2014 Elsevier B.V. All rights reserved.

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  92. Erratum: Multifunctional nanoprobes for nanoscale chemical imaging and localized chemical delivery at surfaces and interfaces (Angewandte Chemie - International Edition (2011) (50) DOI: 10.1002/anie.201102796)

    Takahashi Y., Shevchuk A.I., Novak P., Zhang Y., Ebejer N., Macpherson J.V., Unwin P.R., Pollard A.J., Roy D., Clifford C.A., Shiku H., Matsue T., Klenerman D., Korchev Y.E.

    Angewandte Chemie - International Edition   Vol. 53 ( 28 )   2014.7

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    DOI: 10.1002/anie.201404979

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  93. Nanoscale Cell Surface Topography Imaging using Scanning Ion Conductance Microscopy Reviewed

    Yasufumi Takahashi, Komachi Ito, Xiongwei Wang, Yoshiharu Matsumae, Hirokazu Komaki, Akichika Kumatani, Kosuke Ino, Hitoshi Shiku, Tomokazu Matsue

    ELECTROCHEMISTRY   Vol. 82 ( 5 ) page: 331 - 334   2014.5

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    Nanoscale cell surface topography was visualized using a scanning ion conductance microscope (SICM), where a nanopipette was used as the scanning probe to detect ionic current as feedback signal. SICM was an effective tool for noncontact topographical imaging of live cells, because measurements were performed under physiological conditions. This breakthrough technique opens up a wealth of possible new experiments in membrane and cell biology. (C) The Electrochemical Society of Japan, All rights reserved.

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  94. Densified Electrochemical Sensors Based on Local Redox Cycling between Vertically Separated Electrodes in Substrate Generation/Chip Collection and Extended Feedback Modes Reviewed

    Kosuke Ino, Yusuke Kanno, Taku Nishijo, Hirokazu Komaki, Yuta Yamada, Shinya Yoshida, Yasufumi Takahashi, Hitoshi Shiku, Tomokazu Matsue

    ANALYTICAL CHEMISTRY   Vol. 86 ( 8 ) page: 4016 - 4023   2014.4

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    A new local redox cycling-based electrochemical (LRC-EC) device integrated with many electrochemical sensors has been developed into a small chip device. The LRC-EC chip device was successfully applied for detection of alkaline phosphatase and horseradish peroxidase activity in substrate generation/chip collection (SG/CC) and extended feedback modes, respectively. The new imaging approach with extended feedback mode was particularly effective for sharpening of the image, because this mode uses feedback signals and minimizes the undesired influence of diffusion. The LRC-EC chip device is considered to be a useful tool for bioanalysis.

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  95. SU-8-based Flexible Amperometric Device with IDA Electrodes to Regenerate Redox Species in Small Spaces Reviewed

    Yusuke Kanno, Takehito Goto, Kosuke Ino, Kumi Y. Inoue, Yasufumi Takahashi, Hitoshi Shiku, Tomokazu Matsue

    ANALYTICAL SCIENCES   Vol. 30 ( 2 ) page: 305 - 309   2014.2

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    A flexible sensor based on SU-8 photoresist was fabricated and its electrochemical performance was investigated using cyclic voltammetry. The device consisted of interdigitated array (IDA) electrodes on an SU-8 layer. It exhibited a clear electrochemical response during redox cycling of ferrocenemethanol at the IDA electrodes. Since the device was flexible, it could be inserted into a narrow bent space to monitor electrochemical responses. The observed electrochemical behavior was found to be consistent with that predicted by simulations based on redox compound diffusion.

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  96. Isolation and quantification of messenger RNA from tissue models by using a double-barrel carbon probe Reviewed

    Yuji Nashimoto, Yasufumi Takahashi, Ryosuke Takano, Kosuke Miyashita, Shukuyo Yamada, Kosuke Ino, Hitoshi Shiku, Tomokazu Matsue

    ANALYTICAL AND BIOANALYTICAL CHEMISTRY   Vol. 406 ( 1 ) page: 275 - 282   2014.1

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    In this study, we introduce the double-barrel carbon probe (DBCP)-a simple, affordable microring electrode-which enables the collection and analysis of single cells independent of cellular positioning. The target cells were punctured by utilizing an electric pulse between the two electrodes in DBCP, and the cellular lysates were collected by manual aspiration using the DBCP. The mRNA in the collected lysate was evaluated quantitatively using real-time PCR. The histograms of single-cell relative gene expression normalized to GAPDH were fit to a theoretical lognormal distribution. In the tissue culture model, we focused on angiogenesis to prove that multiple gene expression analysis was available. Finally, we applied DBCP for the embryonic stem (ES) cell-derived cardiomyocytes to substantiate the capability of the probe to collect cells, even from high-volume samples such as spheroids. This method achieves high sensitivity for mRNA at the single-cell level and is applicable in the analysis of various biological samples independent of cellular positioning.

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  97. Electrochemical Nanoprobes for Single-Cell Analysis Reviewed

    Paolo Actis, Sergiy Tokar, Jan Clausmeyer, Babak Babakinejad, Sofya Mikhaleva, Renaud Cornut, Yasufumi Takahashi, Ainara Lopez Cordoba, Pavel Novak, Andrew I. Shevchuck, Jennifer A. Dougan, Sergei G. Kazarian, Petr V. Gorelkin, Alexander S. Erofeev, Igor V. Yaminsky, Patrick R. Unwin, Wolfgang Schuhmann, David Klenerman, Dmitri A. Rusakov, Elena V. Sviderskaya, Yuri E. Korchev

    ACS NANO   Vol. 8 ( 1 ) page: 875 - 884   2014.1

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    The measurement of key molecules in individual cells with minimal disruption to the biological milieu is the next frontier in single-cell analyses. Nanoscale devices are ideal analytical tools because of their small size and their potential for high spatial and temporal resolution recordings. Here, we report the fabrication of disk-shaped carbon nanoelectrodes whose radius can be precisely tuned within the range 5-200 nm. The functionalization of the nanoelectrode with platinum allowed the monitoring of oxygen consumption outside and inside a brain slice. Furthermore, we show that nanoelectrodes of this type can be used to impale individual cells to perform electrochemical measurements within the cell with minimal disruption to cell function. These nanoelectrodes can be fabricated combined with scanning ion conductance microscopy probes, which should allow high resolution electrochemical mapping of species on or in living cells.

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  98. 1P292 Single-cell nanobiopsy to investigate intracellular mRNA localization using scanning ion conductance microscopy(26. Measurements,Poster,The 52nd Annual Meeting of the Biophysical Society of Japan(BSJ2014))

    Nashimoto Yuji, Takahashi Yasufumi, Ino Kosuke, Inoue Y Kumi, Shiku Hitoshi, Matsue Tomokazu

    Seibutsu Butsuri   Vol. 54 ( 1 ) page: S189   2014

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    DOI: 10.2142/biophys.54.S189_4

  99. Nanoscale visualisation of redox activity and Li+ (de)intercalation dynamics at LiFePO4 battery cathodes Reviewed

    Yasufumi Takahashi, Akichika Kumatani, Hirokazu Munakata, Hirotaka Inomata, Komachi Ito, Kosuke Ino, Hitoshi Shiku, Patrick R. Unwin, Yuri E. Korchev, Kiyoshi Kanamura, Tomokazu Matsue

    Nature Commun   ( 5 ) page: 6450 - 6450   2014

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  100. 2P303 Development of Nano Electrochemical Mircoscope for living cell imaging(27. Bioimaging,Poster,The 52nd Annual Meeting of the Biophysical Society of Japan(BSJ2014))

    Takahashi Yasufumi, Mustafa Sen, Matsumae Yoshiharu, Ino Kosuke, Shiku Hitoshi, Matsue Tomokazu

    Seibutsu Butsuri   Vol. 54 ( 1 ) page: S245   2014

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    DOI: 10.2142/biophys.54.S245_3

  101. Droplet array on local redox cycling-based electrochemical (LRC-EC) chip device Reviewed

    Kosuke Ino, Takehito Goto, Yusuke Kanno, Kumi Y. Inoue, Yasufumi Takahashi, Hitoshi Shiku, Tomokazu Matsue

    LAB ON A CHIP   Vol. 14 ( 4 ) page: 787 - 794   2014

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    We have previously reported a local redox cycling-based electrochemical (LRC-EC) system for the incorporation of many electrochemical sensors into a small chip device. In the present study, a new type of LRC-EC chip device was fabricated for the detection of a droplet array. To detect electrochemically redox compounds in droplets, Pt pseudo-reference/counter electrodes were incorporated into the individual sensors of the LRC-EC chip device. Cyclic voltammetry for the LRC-EC chip device with internal Pt pseudo-reference electrodes indicated well-defined voltammograms based on redox cycling for the individual sensor points. The device was successfully applied to the addressable detection of alkaline phosphatase (ALP) activity of HeLa cells in single droplets on the sensor points. Therefore, the LRC-EC chip device is considered to be a useful device for the bioanalysis of droplet systems.

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  102. 3P105 Real-time Monitoring of Membrane Receptor Internalization : Low-Invasive, Quantitative and Single-Cell Level Measurement by SECM(03. Membrane proteins,Poster,The 52nd Annual Meeting of the Biophysical Society of Japan(BSJ2014))

    Matsumae Yoshiharu, Takahashi Yasufumi, Ino Kosuke, Shiku Hitoshi, Matsue Tomokazu

    Seibutsu Butsuri   Vol. 54 ( 1 ) page: S266   2014

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    DOI: 10.2142/biophys.54.S266_3

  103. Local Delivery of Molecules from a Nanopipette for Quantitative Receptor Mapping on Live Cells Reviewed

    Babak Babakinejad, Peter Joensson, Ainara Lopez Cordoba, Paolo Actis, Pavel Novak, Yasufumi Takahashi, Andrew Shevchuk, Uma Anand, Praveen Anand, Anna Drews, Antonio Ferrer-Montiel, David Klenerman, Yuri E. Korchev

    ANALYTICAL CHEMISTRY   Vol. 85 ( 19 ) page: 9333 - 9342   2013.10

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    Using nanopipettes to locally deliver molecules to the surface of living cells could potentially open up studies of biological processes down to the level or single molecules. However, in order to achieve precise and quantitative local delivery it is essential to be able to determine the amount and distribution of the molecules being delivered. In this work, we investigate how the size of the nanopipette, the magnitude of the applied pressure or voltage, which drives the delivery, and the distance to the underlying surface influences the number and spatial distribution of the delivered molecules. Analytical expressions describing the delivery are derived and compared with the results from finite element simulations and experiments on delivery from a 100 nm nanopipette in bulk solution and to the surface of sensory neurons. We then developed a setup for rapid and quantitative delivery to multiple subcellular areas, delivering the molecule capsaicin to stimulate opening of Transient Receptor Potential Vanilloid subfamily member 1 (TRPV1) channels, membrane receptors involved in pain sensation. Overall, precise and quantitative delivery of molecules from nanopipettes has been demonstrated, opening up many applications in biology such as locally stimulating and mapping receptors on the surface of live cells.

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  104. Electrochemical device with interdigitated ring array electrodes for investigating the relationship between cardiomyocyte differentiation from embryonic stem cells and alkaline phosphatase activity Reviewed

    Kosuke Ino, Taku Nishijo, Yusuke Kanno, Fumisato Ozawa, Toshiharu Arai, Yasufumi Takahashi, Hitoshi Shiku, Tomokazu Matsue

    Electrochemistry   Vol. 81 ( 9 ) page: 682 - 687   2013.9

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    A local redox cycling-based electrochemical (LRC-EC) chip device was used to investigate the relationship between cardiomyocyte differentiation from embryonic stem (ES) cells and alkaline phosphatase (ALP) activity. In the LRC-EC chip device, ring-type interdigitated array electrodes were incorporated at n × n measurement points with only 2n bonding pads for external connection. Microwells were also fabricated at each measurement point to trap cell aggregates. To differentiate ES cells into cardiomyocytes, ES cells were three-dimensionally cultured to form simple and cystic embryoid bodies (EBs). ALP activity of these EBs was then detected using the LRC-EC chip device. The electrochemical responses for ALP activity decreased concurrently with the differentiation of ES cells into cardiomyocytes, indicating that an LRC-EC chip device is useful for evaluating cell differentiation. © 2013 The Electrochemical Society of Japan, All rights reserved.

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  105. Fabrication, Characterization, and Functionalization of Dual Carbon Electrodes as Probes for Scanning Electrochemical Microscopy (SECM) Reviewed

    Kim McKelvey, Binoy Paulose Nadappuram, Paolo Actis, Yasufumi Takahashi, Yuri E. Korchev, Tomokazu Matsue, Colin Robinson, Patrick R. Unwin

    ANALYTICAL CHEMISTRY   Vol. 85 ( 15 ) page: 7519 - 7526   2013.8

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    Dual carbon electrodes (DCEs) are quickly, easily, and cheaply fabricated by depositing pyrolytic carbon into a quartz theta nanopipet. The size of DCEs can be controlled by adjusting the pulling parameters used to make the nanopipet. When operated in generation/collection (G/C) mode, the small separation between the electrodes leads to reasonable collection efficiencies of ca. 30%. A three-dimensional finite element method (FEM) simulation is developed to predict the current response of these electrodes as a means of estimating the probe geometry. Voltammetric measurements at individual electrodes combined with generation/collection measurements provide a reasonable guide to the electrode size. DCEs are employed in a scanning electrochemical microscopy (SECM) configuration, and their use for both approach curves and imaging is considered. G/C approach curve measurements are shown to be particularly sensitive to the nature of the substrate, with insulating surfaces leading to enhanced collection efficiencies, whereas conducting surfaces lead to a decrease of collection efficiency. As a proof-of-concept, DCEs are further used to locally generate an artificial electron acceptor and to follow the flux of this species and its reduced form during photosynthesis at isolated thylakoid membranes. In addition, 2-dimensional images of a single thylakoid membrane are reported and analyzed to demonstrate the high sensitivity of G/C measurements to localized surface processes. It is finally shown that individual nanometer-size electrodes can be functionalized through the selective deposition of platinum on one of the two electrodes in a DCE while leaving the other one unmodified. This provides an indication of the future versatility of this type of probe for nanoscale measurements and imaging.

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  106. Carbon-Ag/AgCl probes for detection of cell activity in droplets Reviewed

    Kosuke Ino, Kaoru Ono, Toshiharu Arai, Yasufumi Takahashi, Hitoshi Shiku, Tomokazu Matsue

    Analytical Chemistry   Vol. 85 ( 8 ) page: 3832 - 3835   2013.4

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    In this study, we fabricated a probe consisting of a carbon nanoelectrode and an Ag/AgCl reference electrode for detecting the activity of cells in single droplets. HeLa cells were confined into a single droplet, and the alkaline phosphatase (ALP) activity of the cells was electrochemically measured using the probe inserted into the droplet. The ALP of the confined cells catalyzed the hydrolysis of p-aminophenyl phosphate (PAPP) to yield p-aminophenol (PAP) that gave electrochemical responses. Since the tip of the carbon-Ag/AgCl probe is very small, it is useful for electrochemical analysis of cells using droplets. © 2013 American Chemical Society.

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  107. Electrodeposition of alginate gels for construction of vascular-like structures Reviewed

    Fumisato Ozawa, Kosuke Ino, Yasufumi Takahashi, Hitoshi Shiku, Tomokazu Matsue

    Journal of Bioscience and Bioengineering   Vol. 115 ( 4 ) page: 459 - 461   2013.4

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    In this study, tubular hydrogel structures were constructed via electrodeposition using alginate gels. Electrolysis of water in alginate solutions with calcium carbonate particles induced gel aggregation around Pt wire electrodes, forming tubular alginate gel structures. The simple method is a promising approach for construction of multi-layer tubular hydrogel structures for tissue engineering. © 2012 The Society for Biotechnology, Japan.

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  108. Alginate gel microwell arrays using electrodeposition for three-dimensional cell culture Reviewed

    Fumisato Ozawa, Kosuke Ino, Toshiharu Arai, Javier Ramon-Azcon, Yasufumi Takahashi, Hitoshi Shiku, Tomokazu Matsue

    LAB ON A CHIP   Vol. 13 ( 15 ) page: 3128 - 3135   2013

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    In this study, we developed a novel method for fabricating microwell arrays constructed from alginate gels, and the alginate gel microwells were used for three-dimensional (3D) cell culture. The alginate gel microwells were fabricated on a patterned ITO electrode using alginate gel electrodeposition. Embryonic stem (ES) cells or hepatocellular carcinoma cells (HepG2) were cultured in the alginate gel microwells containing 3T3 cells. During the culture, embryoid bodies (EBs) or HepG2 spheroids were successfully fabricated in the alginate gel microwells. The oxygen consumption of the EBs indicated that they were successfully cultured. Liver-specific gene expressions of the HepG2 spheroids apparently increased by performing 3D co-culture in the microwell arrays with 3T3 cells. These results show that the alginate gel microwells are a useful 3D culture system.

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  109. 1P298 Mapping of neurotransmitter releasing sites using scanning electrochemical ion conductance microscopy(27. Bioimaging,Poster)

    Takahashi Yasufumi, Wang Xiongwe, Ino Kosuke, Shiku Hitoshi, Matsue Tomoakazu

    Seibutsu Butsuri   Vol. 53 ( 1 ) page: S155   2013

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    DOI: 10.2142/biophys.53.S155_3

  110. 1P265 Collection and quantification of messenger RNA from tissue models by double barrel carbon probe(21A. Genome biology: Genome analysis,Poster)

    Nashimoto Yuji, Takahashi Yasufumi, Takano Ryosuke, Miyashita Kosuke, Yamada Shukuyo, Ino Kosuke, Shiku Hitoshi, Matsue Tomokazu

    Seibutsu Butsuri   Vol. 53 ( 1 ) page: S149   2013

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    DOI: 10.2142/biophys.53.S149_6

  111. Evaluation of the differentiation status of single embryonic stem cells using scanning electrochemical microscopy Reviewed

    Yoshiharu Matsumae, Toshiharu Arai, Yasufumi Takahashi, Kosuke Ino, Hitoshi Shiku, Tomokazu Matsue

    CHEMICAL COMMUNICATIONS   Vol. 49 ( 58 ) page: 6498 - 6500   2013

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    The differentiation status of single live embryonic stem (ES) cells was quantitatively evaluated by monitoring the activity of alkaline phosphatase (ALP), an undifferentiation marker of ES cells, using scanning electrochemical microscopy (SECM).

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  112. Bio Sensing and Imaging by Using Mirco/Nano Electrode System

    高橋康史, 珠玖仁, 末永智一

    表面科学   Vol. 34 ( 9 ) page: 488-493 (J-STAGE) - 493   2013

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    The micro/nanoelectrode has unique characteristics, which are not expected for conventional electrodes, such as the capability to perform localized measurements, low double layer charging currents, low ohmic drops, and fast mass transport. Scanning electrochemical microscopy (SECM) with a micro/nanoelectrode for detecting electroactive chemical species and is an effective tool for the investigation of the localized chemical properties of sample surfaces and interfaces. Because SECM has high temporal resolution under physiological conditions, it is particularly well suited for quantitative measurements of chemicals like neurotransmitters, nitric oxide, reactive oxygen species, and oxygen, which are released/consumed by living cells. This article presents an overview of the recent progress of SECM.

    DOI: 10.1380/jsssj.34.488

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  113. Development of a novel combined scanning electrochemical microscope (SECM) and scanning ion-conductance microscope (SICM) probe for soft sample imaging

    Pollard A.J., Faruqui N., Shaw M., Clifford C.A., Takahashi Y., Korchev Y.E., Ebejer N., Macpherson J.V., Unwin P.R., Roy D.

    Materials Research Society Symposium Proceedings   Vol. 1422   page: 13 - 18   2012.12

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    By incorporating a localized heating system within a scanning ion-conductance microscopy (SICM) system, we have performed stable 'hopping-mode' (HPICM) imaging for live cells maintained at temperatures ranging up to human body temperature. This allows the accurate study of cell volume and morphology variation versus temperature over extended periods of time. The integration of SICM with scanning electrochemical microscopy (SECM) provides the simultaneous mapping of electrochemical and topographic information for soft samples, such as live cells. This combined technique overcomes the limitations of resolution and topographical artifacts typically associated with SECM. However, previously reported SECM-SICM probe production required expensive and time-consuming focused ion beam (FIB) methods and produced pipettes that are typically hundreds of nanometers in diameter. We report a simple and rapid production method for SECM-SICM double-barrel probes with apertures down to 20 nm in diameter. The characterization of these SECM-SICM probes using scanning electron microscopy (SEM) imaging, cyclic voltammetry (CV) and Raman spectroscopy is also detailed. These SECM-SICM probes were subsequently used to study the morphology and electrochemical activity of several samples, ranging from hard metallic/insulating samples to live cells. © 2012 Materials Research Society.

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  114. Novel Electrochemical Methodology for Activity Estimation of Alkaline Phosphatase Based on Solubility Difference Reviewed

    Kosuke Ino, Yusuke Kanno, Toshiharu Arai, Kumi Y. Inoue, Yasufumi Takahashi, Hitoshi Shiku, Tomokazu Matsue

    ANALYTICAL CHEMISTRY   Vol. 84 ( 18 ) page: 7593 - 7598   2012.9

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    We propose a novel electrochemical detection system for alkaline phosphatase (ALP) activity using the difference in water and oil solubilities between the substrate, ferrocene ethyl phosphate ester (FcEtOPO(3)(2-)), and the enzymatic product, ferroceneethanol (FcEtOH). In this system, water droplets containing ALP and FcEtOPO(3)(2-) were placed on a Pt disk microelectrode and surrounded by a mineral oil. By the ALP-catalyzed reaction, FcEtOPO(3)(2-) was converted to FcEtOH, which was then transferred to the mineral oil from the water droplets with FcEtOPO(3)(2-) remaining in the water droplets. After partitioning FcEtOH from the water droplets, FcEtOPO(3)(2-) was detected at the Pt disk microelectrode to estimate the ALP activity. Using this novel system, the ALP activity of embryoid bodies was successfully detected. We believe that the present system will be widely applicable to ALP-based bioassays.

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  115. Topographical and electrochemical nanoscale imaging of living cells using voltage-switching mode scanning electrochemical microscopy Reviewed

    Yasufumi Takahashi, Andrew I. Shevchuk, Pavel Novak, Babak Babakinejad, Julie Macpherson, Patrick R. Unwin, Hitoshi Shiku, Julia Gorelik, David Klenerman, Yuri E. Korchev, Tomokazu Matsue

    PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA   Vol. 109 ( 29 ) page: 11540 - 11545   2012.7

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    We describe voltage-switching mode scanning electrochemical microscopy (VSM-SECM), in which a single SECM tip electrode was used to acquire high-quality topographical and electrochemical images of living cells simultaneously. This was achieved by switching the applied voltage so as to change the faradaic current from a hindered diffusion feedback signal (for distance control and topographical imaging) to the electrochemical flux measurement of interest. This imaging method is robust, and a single nanoscale SECM electrode, which is simple to produce, is used for both topography and activity measurements. In order to minimize the delay at voltage switching, we used pyrolytic carbon nanoelectrodes with 6.5-100 nm radii that rapidly reached a steady-state current, typically in less than 20 ms for the largest electrodes and faster for smaller electrodes. In addition, these carbon nanoelectrodes are suitable for convoluted cell topography imaging because the RG value (ratio of overall probe diameter to active electrode diameter) is typically in the range of 1.5-3.0. We first evaluated the resolution of constant-current mode topography imaging using carbon nanoelectrodes. Next, we performed VSM-SECM measurements to visualize membrane proteins on A431 cells and to detect neurotransmitters from a PC12 cells. We also combined VSM-SECM with surface confocal microscopy to allow simultaneous fluorescence and topographical imaging. VSM-SECM opens up new opportunities in nanoscale chemical mapping at interfaces, and should find wide application in the physical and biological sciences.

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  116. 使える解析テクニック!具体例で説明する電気化学測定法 マイクロ電極(3)応用計測事例:電気化学顕微鏡(SECM)‐走査型イオンコンダクタンス顕微鏡(SICM)複合システムの開発

    高橋康史, 珠玖仁, 末永智一

    電気化学および工業物理化学   Vol. 80 ( 4 ) page: 271 - 275   2012.4

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  117. Local Redox-Cycling-Based Electrochemical Chip Device with Deep Microwells for Evaluation of Embryoid Bodies Reviewed

    Kosuke Ino, Taku Nishijo, Toshiharu Arai, Yusuke Kanno, Yasufumi Takahashi, Hitoshi Shiku, Tomokazu Matsue

    ANGEWANDTE CHEMIE-INTERNATIONAL EDITION   Vol. 51 ( 27 ) page: 6648 - 6652   2012

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  118. Electrochemical detection for dynamic analyses of a redox component in droplets using a local redox cycling-based electrochemical (LRC-EC) chip device Reviewed

    Kosuke Ino, Yusuke Kanno, Taku Nishijo, Takehito Goto, Toshiharu Arai, Yasufumi Takahashi, Hitoshi Shiku, Tomokazu Matsue

    CHEMICAL COMMUNICATIONS   Vol. 48 ( 68 ) page: 8505 - 8507   2012

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    This report describes the electrochemical detection of a redox component in droplets using a local redox cycling-based electrochemical (LRC-EC) chip device consisting of 256 sensors. The time-course analyses showed that the redox compound in the droplet was dynamically changed during droplet evaporation or mass transfer through a water/oil interface.

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  119. Influence of Tip Size on Single Yeast Cell Imaging Using Scanning Electrochemical Microscopy Reviewed

    Kuniaki Nagamine, Yasufumi Takahashi, Kosuke Ino, Hitoshi Shiku, Tomokazu Matsue

    ELECTROANALYSIS   Vol. 23 ( 5 ) page: 1168 - 1174   2011.5

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    The influence of the tip reaction on the substrate generation/tip collection mode SECM imaging of a single yeast cell was investigated by using various sizes of probe electrodes in mu m-nm scales because the tip reaction would disturb the concentration profile of intracellular enzyme reactant formed around the cell. GC mode measurements of a single yeast cell were performed using a dual mediator system with lipophilic menadione and hydrophilic ferricyanide. We found downscaling of the tip size enabled quantitative SECM imaging of a single cell in GC mode without disturbing the concentration profile of the mediator formed around the cell by the tip reaction.

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  120. Realizing the biological and biomedical potential of nanoscale imaging using a pipette probe Reviewed

    Andrew I. Shevchuk, Pavel Novak, Yasufumi Takahashi, Richard Clarke, Michele Miragoli, Babak Babakinejad, Julia Gorelik, Yuri E. Korchev, David Klenerman

    NANOMEDICINE   Vol. 6 ( 3 ) page: 565 - 575   2011.4

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    Cells naturally operate on the nanoscale level, with molecules combining together to form complex molecular machines, which can work together to enable normal cell function or go wrong as in the case of many diseases. Visualizing these key processes on the nanoscale has been difficult and two main approaches have been used to date; nanometer resolution imaging of fixed cells using electron microscopy, or imaging live cells using optical or fluorescence microscopy, with a resolution of a few hundred nanometers. Scanning probe microscopy has the potential to allow live cells to be imaged at nanoscale resolution and a noncontact method based on the use of a nanopipette probe has been developed over the last 10 years that allows both topographic and functional imaging. The rapid progress in this area of research over the last 4 years is reviewed in this article, which shows that imaging of complex cellular structures and tissues is now possible and that these methods are now sufficiently mature to provide new insights into important diseases.

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  121. Multifunctional Nanoprobes for Nanoscale Chemical Imaging and Localized Chemical Delivery at Surfaces and Interfaces Reviewed

    Yasufumi Takahashi, Andrew I. Shevchuk, Pavel Novak, Yanjun Zhang, Neil Ebejer, Julie V. Macpherson, Patrick R. Unwin, Andrew J. Pollard, Debdulal Roy, Charles A. Clifford, Hitoshi Shiku, Tomokazu Matsue, David Klenerman, Yuri E. Korchev

    ANGEWANDTE CHEMIE-INTERNATIONAL EDITION   Vol. 50 ( 41 ) page: 9638 - 9642   2011

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  122. Electrochemical detection of receptor-mediated endocytosis by scanning electrochemical microscopy Reviewed

    Yasufumi Takahashi, Takeshi Miyamoto, Hitoshi Shiku, Kosuke Ino, Tomoyuki Yasukawa, Ryutaro Asano, Izumi Kumagai, Tomokazu Matsue

    PHYSICAL CHEMISTRY CHEMICAL PHYSICS   Vol. 13 ( 37 ) page: 16569 - 16573   2011

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    We report a scanning electrochemical microscopy (SECM)-based receptor-mediated endocytosis detection method. Epidermal growth factor receptor (EGFR), which is one of the key membrane proteins associated with cancer, was used as a model for receptor-mediated endocytosis. EGFR molecules on the outer cell membrane were detected by SECM by using alkaline phosphatase (ALP) as a labeling enzyme. Since SECM detected the ALP activity on the outer membrane, the procedure helped discriminate the EGFR on the outer membrane from the intracellular EGFR involved in endocytosis. SECM showed a marked decrease in the current responses generated due to ALP activity by 93% on addition of the epidermal growth factor, indicating clearly that EGF triggered the endocytosis, which led to the withdrawal of most EGFRs from the outer membrane.

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  123. Reporter gene expression at single-cell level characterized with real-time RT-PCR, chemiluminescence, fluorescence, and electrochemical imaging Reviewed

    Hitoshi Shiku, Daisuke Okazaki, Junya Suzuki, Yasufumi Takahashi, Tatsuya Murata, Hidetaka Akita, Hideyoshi Harashima, Kosuke Ino, Tomokazu Matsue

    FEBS LETTERS   Vol. 584 ( 18 ) page: 4000 - 4008   2010.9

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    mRNA from single cells was quantified using real-time RT-PCR after recording the address and reporter protein activity with chemiluminescence, fluorescence, and electrochemical techniques, using luciferase, green fluorescent protein, and secreted alkaline phosphatase. mRNA copy number ranging from below 103 to 107 in single cells showed a lognormal distribution for both externally introduced reporter genes and internally expressed genes. The fluctuation in the gene expression decreased with the increase of the number of cells picked but did not decrease with the increase of mRNA copy number per cell. We found that the correlation coefficients for mRNA and protein expression in logarithmic plot at single-cell level were much lower than 1.00. (c) 2010 Federation of European Biochemical Societies. Published by Elsevier B.V. All rights reserved.

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  124. Simultaneous Noncontact Topography and Electrochemical Imaging by SECM/SICM Featuring Ion Current Feedback Regulation Reviewed

    Yasufumi Takahashi, Andrew I. Shevchuk, Pavel Novak, Yumi Murakami, Hitoshi Shiku, Yuri E. Korchev, Tomokazu Matsue

    JOURNAL OF THE AMERICAN CHEMICAL SOCIETY   Vol. 132 ( 29 ) page: 10118 - 10126   2010.7

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    We described a hybrid system of scanning electrochemical microscopy (SECM) and scanning ion conductance microscopy (SICM) with ion current feedback nanopositioning control for simultaneous imaging of noncontact topography and spatial distribution of electrochemical species. A nanopipette/nanoring electrode probe provided submicrometer resolution of the electrochemical measurement on surfaces with complex topology. The SECM/SICM probe had an aperture radius of 220 nm. The inner and outer radii of the SECM Au nanoring electrode were 330 and 550 nm, respectively. Characterization of the probe was performed with scanning electron microscopy (SEM), cyclic voltammetry (CV), and approach curve measurements. SECM/SICM was applied to simultaneous imaging of topography and electrochemical responses of enzymes (horse radish peroxidase (HRP) and glucose oxidase (GOD)) and single live cells (A6 cells, superior cervical ganglion (SCG) cells, and cardiac myocytes). The measurements revealed the distribution of activity of the enzyme spots on uneven surfaces with submicrometer resolution. SECM/ SICM acquired high resolution topographic images of cells together with the map of electrochemical signals. This combined technique was also applied to the evaluation of the permeation property of electroactive species through cellular membranes.

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  125. Topographic imaging of convoluted surface of live cells by scanning ion conductance microscopy in a standing approach mode Reviewed

    Yasufumi Takahashi, Yumi Murakami, Kuniaki Nagamine, Hitoshi Shiku, Shigeo Aoyagi, Tomoyuki Yasukawa, Makoto Kanzaki, Tomokazu Matsue

    PHYSICAL CHEMISTRY CHEMICAL PHYSICS   Vol. 12 ( 34 ) page: 10012 - 10017   2010

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    Scanning ion conductance microscopy (SICM) using a nanopipette as a probe and ionic current as a feedback signal was introduced as a novel technique to study live cells in a physiological environment. To avoid contact between the pipette tip and cells during the conventional lateral scanning mode, we adopted a standing approach (STA) mode in which the probe was moved vertically to first approach and then retracted from the cell surface at each measurement point on an XY plane. The STA mode ensured non-contact imaging of the topography of live cells and for a wide range of uneven substrates (500 x 300 mu m to 5 x 5 mu m). We also used a field-programmable gate array (FPGA) board to enhance feedback distance regulation. FPGA dramatically increased the feedback speed and decreased the imaging time (450 s per image) with enhanced accuracy and quality of live cell images. To evaluate the potential of the STA mode for SICM, we carried out imaging of a convoluted surface of live cell in various scan ranges and estimated the spatial resolutions of these images.

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  126. Electrochemical characterization of enzyme and immunoglobulin G patterned using microcontact printing Reviewed

    Hitoshi Shiku, Ayako Kumagai, Hong Qun Luo, Yasufumi Takahashi, Tomoyuki Yasukawa, Hiroshi Yamada, Tomokazu Matsue

    Electrochemistry   Vol. 78 ( 2 ) page: 122 - 125   2010

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    Microcontact printing (μCP) with various proteins has been widely applied to biosensors and cell biology research. However, the mechanism of protein patterning in the μCP process is not clear in detail We have electrochemically estimated enzyme concentration on glass slide patterned with μCP technique. We also estimated the enzyme concentration at the surface of poly(dimethylsiloxane) (PDMS), which corresponded to the enzyme activity at the PDMS stamp just before μCP. Our result suggested that it was possible to transfer enzyme monolayer from PDMS to glass surfaces with 100% efficiency with μCP. Immunoglobulin G (IgG) patterned with μCP was also characterized by tagging with enzyme labeled anti-IgG. Scanning electrochemical microscopy (SECM) image was obtained to visualize line and space pattern of IgG monolayer.

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  127. Transfected Single-Cell Imaging by Scanning Electrochemical Optical Microscopy with Shear Force Feedback Regulation Reviewed

    Yasufumi Takahashi, Hitoshi Shiku, Tatsuya Murata, Tomoyuki Yasukawa, Tomokazu Matsue

    ANALYTICAL CHEMISTRY   Vol. 81 ( 23 ) page: 9674 - 9681   2009.12

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    Gene-transfected single HeLa cells were characterized using a scanning electrochemical/optical microscope (SECM/OM) system with shear-force-based probe-sample distance regulation to simultaneously capture electrochemical, fluorescent, and topographic images. The outer and inner states of single living cells were obtained as electrochemical and fluorescent signals, respectively, by using an optical fiber-nanoelectrode probe. A focused ion beam (FIB) was used to mill the optical aperture and the ring electrode at the probe apex (the inner and outer radii of the ring electrode were 3 7 and 112 nm, respectively). To apply an appropriate shear force between the probe tip and the living cell surface, we optimized the amplitude of oscillation of the tuning fork to which the probe was attached. Field-programmable gate arrays (FPGA) were adopted to drastically increase the feedback speed of the tip-sample distance regulation, shorten the scanning time for imaging, and enhance the accuracy and quality of the living cell images. In employing these improvements, we simultaneously measured the cellular expression activity of both secreted alkaline phosphatase outside and GFP inside by using the SECM/OM with shear force distance regulation.

    DOI: 10.1021/ac901796r

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  128. Three dimensional microelectrode array device integrating multi-channel microfluidics to realize manipulation and characterization of enzyme-immobilized polystyrene beads Reviewed

    Ryouta Kunikata, Yasufumi Takahashi, Masahiro Koide, Tomoaki Itayama, Tomoyuki Yasukawa, Hitoshi Shiku, Tomokazu Matsue

    SENSORS AND ACTUATORS B-CHEMICAL   Vol. 141 ( 1 ) page: 256 - 262   2009.8

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    We microfabricated a novel device consisting of a 4 x 4 array microchamber sandwiched with the two microband electrode array. This device allows dielectrophoretic (DEP) manipulation of microbeads to introduce into and release out a certain address of the V-shaped microchamber, by applying AC voltage (10 V(pp), 10 kHz) on the basis of DEP forces. The design and the position of the two electrodes (row and column electrodes) at each microchamber were optimized by simulation based on a finite element method. More importantly, electrochemical generation-collection measurement was possible to evaluate enzymatic activity. After microbeads immobilized with glucose oxidase (GOD) was entrapped in the V-shaped microchamber with DEP, a measuring solution containing 3 mM ferrocenemethanol (FcCH(2)OH) and 0.1 M glucose was introduced. The medium in the V-shaped microwell was immediately exchanged into the measuring solution whereas microbeads stayed within the microwell without applying DEP voltage, because the flow within the microchamber was isolated from that of the main channel. Then the potential of the row and column electrodes were set at 0.5 and 0.1 V vs Ag/AgCl. The GOD activity can be monitored as the decrease in the [FcCh(2)OH](+) reduction current. (C) 2009 Elsevier B.V. All rights reserved.

    DOI: 10.1016/j.snb.2009.05.028

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  129. Electrochemical Detection of Epidermal Growth Factor Receptors on a Single Living Cell Surface by Scanning Electrochemical Microscopy Reviewed

    Yasufumi Takahashi, Takeshi Miyamoto, Hitoshi Shiku, Ryutaro Asano, Tomoyuki Yasukawa, Izumi Kumagai, Tomokazu Matsue

    ANALYTICAL CHEMISTRY   Vol. 81 ( 7 ) page: 2785 - 2790   2009.4

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    A membrane protein on the surface of a single living mammalian cell was imaged by scanning electrochemical microscopy (SECM). The epidermal growth factor receptor (EGFR) is one of the key membrane proteins associated with cancer. It elicits a wide range of cell-type-specific responses, leading to cell proliferation, differentiation, apoptosis, and migration. To estimate EGFR expression levels by SECM, EGFR was labeled with alkaline phosphatase (ALP) via an antibody. The oxidation current of PAP (p-aminophenol) produced by the ALP-catalyzed reaction was monitored to estimate the density of cell surface EGFR. EGFR measurement by SECM has three advantages. First, a single adhesion cell can be measured without peeling it from the culture dish; second, it is possible to optimize labeling antibody concentrations by using living cells because detection of faradaic current is suitable for quantitative estimation in situ; and third, SECM measurements afford information on the expression state at the cell membrane at the single-cell level. In this study, we optimized the concentration of labeling antibody for EGFR at the cell surface and confirmed distinct differences in EGFR expression levels among three types of cells. SECM measurements were compatible with the results of flow cytometry.

    DOI: 10.1021/ac900195m

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  130. A microfluidic dual capillary probe to collect messenger RNA from adherent cells and spheroids Reviewed

    Hitoshi Shiku, Takeshi Yamakawa, Yuji Nashimoto, Yasufumi Takahashi, Yu-suke Torisawa, Tomoyuki Yasukawa, Takahiro Ito-Sasaki, Masaki Yokoo, Hiroyuki Abe, Hideki Kambara, Tomokazu Matsue

    ANALYTICAL BIOCHEMISTRY   Vol. 385 ( 1 ) page: 138 - 142   2009.2

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    Collection of bioanalytes from single cells is still a challenging technology despite the recent progress in many integrated microfluidic devices. A microfluidic dual capillary probe was prepared from a theta (theta)-shaped glass capillary to analyze messenger RNA (mRNA) from adherent cells and spheroids. The cell lysis buffer Solution was introduced from the injection aperture, and the cell-lysed solution from the aspiration aperture was collected for further mRNA analysis based on reverse transcription real-time PCR. The cell lysis buffer can be introduced at any targeted cells and never spilled out of the targeted area by using the microfluidic dual capillary probe because laminar flow was locally formed near the probe under the optimized injection/aspiration flow rates. This method realizes the sensitivity of mRNA at the single cell level and the identification of the cell types on the basis of the relative gene expression profiles. (C) 2008 Elsevier Inc. All rights reserved.

    DOI: 10.1016/j.ab.2008.10.039

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  131. Electrochemical Gene-Function Analysis for Single Cells with Addressable Microelectrode/Microwell Arrays Reviewed

    Zhenyu Lin, Yasufumi Takahashi, Tatsttya Murata, Michiaki Takeda, Kosuke Ino, Hitoshi Shiku, Tomokazu Matsue

    ANGEWANDTE CHEMIE-INTERNATIONAL EDITION   Vol. 48 ( 11 ) page: 2044 - 2046   2009

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    Language:English   Publishing type:Research paper (scientific journal)   Publisher:WILEY-V C H VERLAG GMBH  

    DOI: 10.1002/anie.200805743

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  132. Entrapment and measurement of a biologically functionalized microbead with a microwell electrode Reviewed

    Ching-Yu Chang, Yasufumi Takahashi, Tatsuya Murata, Hitoshi Shiku, Hsien-Chang Chang, Tomokazu Matsue

    LAB ON A CHIP   Vol. 9 ( 9 ) page: 1185 - 1192   2009

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    A chip with integrated electrophoretic and electrochemical systems was developed to manipulate either an individual microbead or a cell inside a microwell electrode (MWE) for electrochemical measurement. The optimal MWE geometry (30 mm diameter and 25 mm depth) was designed to accommodate the micro particles according to the simulated results. A chip device was sequentially built from a slide patterned with Pt electrodes, an adhesive tape defined with a flow channel (200 mm in width and 25 mm in height), and an indium tin oxide (ITO) cover. The MWE not only generated an active electrophoretic force to trap the particle but also provided a low flow velocity area (LFVA) to stabilize the trapped bead or cell in a continuous flow. Scanning electrochemical microscopy (SECM) theory was employed to explain the electrochemical behaviors of the MWE. An enhanced current was confirmed as the redox recycling effect on the conductive ITO cover. The catalytic reaction of an individual alkaline phosphatase coated microbead (ALP-bead) was electrochemically detected with the MWE after being trapped. The ALP on the trapped ALP-bead catalyzed the hydrolysis of p-aminophenylphosphate (PAPP) to p-aminophenol ( PAP), and then a decaying amperogram (+0.3 V vs. Ag/AgCl) due to a tiny PAP quantity around the MWE was observed.

    DOI: 10.1039/b817705h

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  133. An addressable microelectrode array for electrochemical detection Reviewed

    Zhenyu Lin, Yasufumi Takahashi, Yuusuke Kitagawa, Taizo Umemura, Hitoshi Shiku, Tomokazu Matsue

    ANALYTICAL CHEMISTRY   Vol. 80 ( 17 ) page: 6830 - 6833   2008.9

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    Column and row electrodes on two different glass substrates were orthogonally arranged in order to assemble an addressable microelectrode device for the purpose of comprehensive electrochemical detection. Amperometric signal at the individual crossing point of the column and row electrodes was detected separately on the basis of redox cycling of localized electroactive species occurring between the electrodes. The addressable microelectrode device was simple and could be easily assembled; however, it comprised as many as 10 x 10 addressable detection points on a single chip. The basic electrochemical performance of the device was investigated by using the ferricyanide/ferrocyanide redox couple. Electrochemical responses at 100 individual points could be collected within 22 s. The present device was successfully used for imaging the spots of alkaline phosphatase on the array substrate. The results indicate that the device can be applied to comprehensive and higb-throughput detection and imaging of biochemical species.

    DOI: 10.1021/ac801389d

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  134. 立体格子電極ウェルアレイデバイスによる微粒子の捕捉と電気化学検出

    梅村 太三, 珠玖 仁, 高橋 康史, 伊野 浩介, 末永 智一

    化学工学会 研究発表講演要旨集   Vol. 2008   page: 950 - 950   2008

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    DOI: 10.11491/scej.2008f.0.950.0

  135. Microcontact printed diaphorase monolayer on glass characterized by atomic force microscopy and scanning electrochemical microscopy Reviewed

    Hong Qun Luo, Hitoshi Shiku, Ayako Kumagai, Yasufumi Takahashi, Tomoyuki Yasukawa, Tomokazu Matsue

    ELECTROCHEMISTRY COMMUNICATIONS   Vol. 9 ( 11 ) page: 2703 - 2708   2007.11

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    Micropatterns of diaphorase (Dp) were fabricated on glass substrates by the microcontact printing (mu CP) method and characterized with atomic force microscopy (AFM) and scanning electrochemical microscopy (SECM). AFM images of the printed samples revealed that the mean height of the Dp patterns was 3-5 nm, indicating the formation of a monolayer pattern. The Dp molecules on the surface organized themselves into two-dimensional arrays. We used two kinds of inking solutions: Dp-phosphate buffer solution (PBS) (pH 7.0) and Dp-PBS (pH 7.0) with glutaraldehyde (GA, 1% v/v) as a cross-linking reagent. Although the AFM imaging showed high-quality Dp monolayer patterns in both cases, SECM measurements indicated that the enzymatic activity of Dp was almost lost when Dp-PBS with GA was used as the inking solution, whereas clear enzymatic activity was found when Dp-PBS was used. (C) 2007 Elsevier B.V. All rights reserved.

    DOI: 10.1016/j.elecom.2007.08.024

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  136. Measurement of gene expression from single adherent cells and spheroids collected using fast electrical lysis Reviewed

    Yuji Nashimoto, Yasufumi Takahashi, Takeshi Yamakawa, Yu-Suke Torisawa, Tomoyuki Yasukawa, Takahiro Ito-Sasaki, Masaki Yokoo, Hiroyuki Abe, Hitoshi Shiku, Hideki Kambara, Tomokazu Matsue

    ANALYTICAL CHEMISTRY   Vol. 79 ( 17 ) page: 6823 - 6830   2007.9

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    The cytosol of a single adherent cell was collected by the electrical cell lysis method with a Pt-ring capillary probe, and the cellular messenger RNA (mRNA) was analyzed at a single-cell level. The ring electrode probe was positioned 20 pin above the cultured cells that formed a monolayer on an indium-tin oxide (ITO) electrode, and an electric pulse with a magnitude of 40 V was applied for 10,us between the probe and the ITO electrodes in an isotonic sucrose solution. Immediately after the electric pulse, less than 1 mu L of the lysed solution was collected using a microinjector followed by RNA purification and first strand cDNA synthesis. Real-time PCR was performed to quantify the copy numbers of mRNA encoding glyceraldehyde-3-phosphate dehydrogenase (GAPDH) expression inside the single cell. The average copy numbers of GAPDH mRNA collected by the electrical cell lysis method were found to be comparable to those obtained by a simple capillary suction method. Although single-cell analysis has already been demonstrated, we have shown for the first time that the fast electrical cell lysis can be used for quantitative mRNA analysis at the singlecell level. This electrical cell lysis method was further applied for the analysis of mRNA obtained from single spheroids-die aggregated cellular masses formed during the three-dimensional culture-as a model system to isolate small cellular clusters from tissues and organs.

    DOI: 10.1021/ac071050q

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  137. Dual - Capillary micro - Fluidic probe to collect mRNA from a single adherent cells Reviewed

    H. Shiku, T. Yamakawa, Y. Nashimoto, Y. Takahashi, Y. Torisawa, T. Yasukawa, T. Ito-Sasaki, M. Yokoo, H. Abe, H. Kambara, T. Matsue

    PROGRESS ON POST-GENOME TECHNOLOGIES     page: 61 - 64   2007

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    We have applied the microfluidic probe (MFP) to collect mRNA from single adherent cells. The probe prepared from a theta (theta-shaped capillary can be positioned at any target single adherent cell. The cell lysis buffer was introduced from the injection aperture, and the cell-lysed solution was recovered from the aspiration aperture for further mRNA analysis based on reverse transcription (RT) real-time PCR. This method achieves not only sensitivity at the single cell level but identifies the differences in cell types based on the relative gene expression profiles. The collection efficiency for mRNA was quantitatively evaluated using real-time PCR.

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  138. Topographic, electrochemical, and optical images captured using standing approach mode scanning electrochemical/optical microscopy. Reviewed

    Takahashi Y, Hirano Y, Yasukawa T, Shiku H, Yamada H, Matsue T

    Langmuir : the ACS journal of surfaces and colloids   Vol. 22 ( 25 ) page: 10299 - 10306   2006.12

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    DOI: 10.1021/la0611763

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  139. Protein Patterning Techniques and Analysis of Interfaces Phenomenon

    高橋康史, 珠玖仁, 安川智之, 末永智一

    表面科学   Vol. 27 ( 10 ) page: 613 - 616   2006.10

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    DOI: 10.1380/jsssj.27.613

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Books 5

  1. Local Electrochemical Characterization Using Scanning Electrochemical Cell Microscopy

    Makarova M.V., Takahashi Y.

    Bioanalytical Reviews  2022 

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    Scanning electrochemical cell microscopy (SECCM) is a unique tool for nanoscale electrochemical imaging for characterizing sample reactivity. It uses a mobile meniscus state electrochemical cell between the nanopipette and the sample. The chapter describes the method setup and principles as well as its reported applications in materials sciences. SECCM was successfully used to image various types of reactions such as hydrogen/oxygen evolution, oxygen/CO2 reduction, corrosion, photocatalysis, and charge/discharge processes in battery materials. The studied objects included carbon phases: diamond and graphite with their derivatives; polymers; transitional metal dichalcogenides; metals; Li complex oxides. SECCM demonstrated site-dependent electrochemical activity, particularly, the role of defects and grain boundaries. Combination of SECCM with EBSD provided the information about the correlation between electrochemical reactivity and terminating facet in multiple kinds of 3D materials. Moreover, SECCM can be used not only to image but also to build new patterned on-surface (sub)microstructures by loading the precursors into the pipette or by site-dependent electrooxidation/reduction of the surface. Thus, the advantages and goals of SECCM for various applications are described in the chapter.

    DOI: 10.1007/11663_2021_12

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  2. 生きてるものは全部観る! イメージングの選び方・使い方100+

    高橋 康史( Role: Contributor ,  45.原子間力顕微鏡 ⅱ.走査型イオンコンダクタンス顕微鏡―生細胞の形状と機能をナノスケールで可視化)

    羊土社  2018.12 

  3. Ion conductance probe microscopy-molecular resolution

    Zhou Y., Fukuma T., Takahashi Y.

    Encyclopedia of Interfacial Chemistry: Surface Science and Electrochemistry  2018.1  ( ISBN:9780128097397

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    Scanning ion-conductance microscopy (SICM) is a nanopipette-based technique that has been widely used in noncontact topography imaging, particularly for imaging cell surfaces. Recent studies have considerably improved the spatiotemporal resolution of SICM based on miniaturization of the probe and development of new scanning mode. In addition, SICM can provide nanoscale functional information of sample surface alone or combined with other techniques. In this article, we focus on these functional imaging and sensing applications of SICM. First, we highlight the combination of SICM with electrochemical sensing. For example, when SICM is combined with scanning electrochemical microscopy, the surface topography and chemical activity can be imaged simultaneously. Second, we introduce SICM for surface-charge mapping and other nanopore-based platforms. The ion current rectification effect that is dependent on the interaction of transported ions with the surface charge of both nanopipette itself and substrate have been used for these applications. When SICM is combined with chemical modified nanopipettes, ion channels, proteins, as well as intracellular pH and glucose can be detected with high spatial resolution. Finally, we discuss SICM probes used for the nanoscale extraction of intracellular molecules from single living cells. The extracted samples can be used to access cell functions by molecular biology techniques.

    DOI: 10.1016/B978-0-12-409547-2.13510-3

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  4. Nanobiosensors and Nanobioanalyses

    Mun'delanji C. Vestergaard, Kagan Kerman, I-Ming Hsing, Eiichi Tamiya

    Springer  2015.3  ( ISBN:4431551891

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    Total pages:379  

    ASIN

  5. バイオ電気化学の実際―バイオセンサ・バイオ電池の実用展開 (CMCテクニカルライブラリー 456 バイオテクノロジーシリーズ)

    池田篤治

    シーエムシー出版  2013.4  ( ISBN:4781307159

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    Total pages:314  

    ASIN

MISC 35

  1. Alkaline Phosphatase-based Electrochemical Analysis for Point-of-Care Testing

    Yusuke Kanno, Yuanshu Zhou, Takeshi Fukuma, Yasufumi Takahashi

    Electroanalysis   Vol. 34 ( 2 ) page: 161 - 167   2022.2

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    Point-of-care testing (POCT) devices have evolved to provide beneficial information about an individual's health whenever needed. Enzyme-based analytical devices have facilitated the highly selective detection of numerous biological molecules and ions. Enzymes are commonly used as the tags of recognition components, such as antibodies, to generate and amplify detection signals. Particularly, alkaline phosphatase (ALP) is one of the most widely used enzymes because of its high turnover number and low cost. Rapid response time and the incorporation of many sensors fabricated by micro/nano processing technologies are the advantages in using electrochemical devices as analytical tools. Therefore, ALP-based electrochemical devices have potential applications for more practical POCT platforms. This review summarizes recent research progress of ALP-based electrochemical devices for POCT. In addition to ALP substrates, the application of ALP-based immunosensors, aptasensors, and DNAzyme sensors are discussed.

    DOI: 10.1002/elan.202100294

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  2. 高速走査型イオンコンダクタンス顕微鏡による細胞表面の微小構造動態の非侵襲測定

    井田大貴, 高橋康史, 珠玖仁, 末永智一

    第1回細胞生物若手の会     2015.6

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  3. CMOS型電気化学デバイスを用いた神経細胞塊から放出される神経伝達物質のイメージング

    阿部博弥, 伊野浩介, LI Chen‐Zhong, 菅野祐介, 井上久美, 國方亮太, 須田篤史, 松平昌昭, 高橋康史, 珠玖仁, 末永智一

    電気化学会大会講演要旨集(CD-ROM)   Vol. 82nd   page: ROMBUNNO.PS31   2015.3

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  4. 走査型イオンコンダクタンス顕微鏡を用いたセネッセンス細胞の表面形状測定

    井田大貴, 高橋康史, 松前義治, 伊野浩介, 珠玖仁, 末永智一

    電気化学会大会講演要旨集(CD-ROM)   Vol. 82nd   page: ROMBUNNO.3M02   2015.3

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  5. マウス胚様体血管新生モデルにおける局所遺伝子解析

    伊藤秀矩, 梨本裕司, 高橋康史, 伊野浩介, 珠玖仁, 末永智一

    電気化学会大会講演要旨集(CD-ROM)   Vol. 82nd   page: ROMBUNNO.1M02   2015.3

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  6. ナノ電気化学セル顕微鏡:有機ゲルピペットの電池材料評価への応用

    熊谷明哉, 高橋康史, 猪又宏貴, 白木将, 山本邦子, 春田正和, 伊野浩介, 珠玖仁, 一杉太郎, 末永智一

    電気化学会大会講演要旨集(CD-ROM)   Vol. 82nd   page: ROMBUNNO.PBT03   2015.3

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  7. ナノ電気化学セル顕微鏡:有機ゲルピペットを用いた局所電気化学測定条件の検討

    熊谷明哉, 高橋康史, 猪又宏貴, 白木将, 山本邦子, 春田正和, 伊野浩介, 珠玖仁, 一杉太郎, 末永智一

    応用物理学会春季学術講演会講演予稿集(CD-ROM)   Vol. 62nd   page: ROMBUNNO.14A-D9-4   2015.2

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  8. SICM-Based Nanodelivery System for Local TRPV1 Stimulation

    Ainara Lopez-Cordoba, Peter Joensson, Babak Babakinejad, Paolo Actis, Pavel Novak, Takahashi Yasufumi, Andrew Shevchuck, Uma Anand, Praveen Anand, Anna Drews, Antonio Ferrer-Montiel, David Klenerman, Yuri Korchev

    BIOPHYSICAL JOURNAL   Vol. 108 ( 2 ) page: 332A - 332A   2015.1

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  9. ナノスケール形状の非侵襲測定を可能にする高速走査型イオンコンダクタンス顕微鏡

    井田大貴, 高橋康史, 高橋康史, 高橋康史, 珠玖仁, 末永智一, 末永智一

    日本生化学会大会(Web)   Vol. 88th   page: 4T19L-08(3P0896) (WEB ONLY)   2015

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  10. LiFePO<sub>4</sub>正極薄膜材料表面のイオン電流応答における結晶粒・粒界の影響

    熊谷明哉, 高橋康史, 猪又宏貴, 白木将, 山本邦子, 春田正和, 伊野浩介, 珠玖仁, 一杉太郎, 末永智一

    電池討論会講演要旨集   Vol. 55th   page: 252   2014.11

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  11. 界面イオン伝導顕微鏡を利用した充放電特性の局所イメージング

    高橋康史, 熊谷明哉, 猪俣宏貴, 棟方裕一, 伊野浩介, 珠玖仁, 金村聖志, 末永智一

    電池討論会講演要旨集   Vol. 55th   page: 251   2014.11

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  12. マウスES細胞の神経細胞分化誘導系における呼吸活性と網羅的遺伝子解析

    珠玖仁, 新井俊陽, ZHOU Y, 高橋康史, 伊野浩介, 井上久美, 末永智一

    電気化学秋季大会講演要旨集   Vol. 2014   page: 202   2014.9

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  13. 界面イオン伝導顕微鏡を利用した充放電特性のリアルタイムイメージング

    高橋康史, 熊谷明哉, 猪俣宏貴, 棟方裕一, 伊野浩介, 珠玖仁, 金村聖志, 末永智一

    電気化学秋季大会講演要旨集   Vol. 2014   page: 245   2014.9

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  14. 液絡構造を排した変換ストリッピングデバイスによる高感度エンドトキシン検出法の開発

    高野真一朗, 井上(安田)久美, 高橋康史, 伊野浩介, 珠玖仁, 末永智一

    電気化学秋季大会講演要旨集   Vol. 2014   page: 225   2014.9

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  15. ES細胞を用いた血管新生モデルの構築と局所遺伝子解析

    伊藤秀矩, 梨本裕司, 高橋康史, 伊野浩介, 珠玖仁, 末永智一

    化学系学協会東北大会プログラムおよび講演予稿集   Vol. 2014   page: 90   2014.9

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  16. 走査型イオンコンダクタンス顕微鏡を用いたクラスリンピットの連続イメージング

    井田大貴, 松前義治, 高橋康史, 伊野浩介, 珠玖仁, 末永智一

    化学系学協会東北大会プログラムおよび講演予稿集   Vol. 2014   page: 91   2014.9

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    J-GLOBAL

  17. 神経細胞から分泌されるシグナル物質の解析に向けた電気化学デバイスの開発

    阿部博弥, 菅野祐介, 伊野浩介, 高橋康史, 井上(安田)久美, 珠玖仁, LI Chenzhong, 末永智一

    化学系学協会東北大会プログラムおよび講演予稿集   Vol. 2014   page: 90   2014.9

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    J-GLOBAL

  18. 界面イオン伝導顕微鏡を用いたLiイオン電池電極表面におけるLi挿入脱離特性のマッピング

    猪又宏貴, 熊谷明哉, 高橋康史, 棟方裕一, 珠玖仁, 金村聖志, 末永智一

    化学系学協会東北大会プログラムおよび講演予稿集   Vol. 2014   page: 206   2014.9

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    J-GLOBAL

  19. ナノ電気化学顕微鏡を用いたケミカルマッピング

    高橋康史

    化学系学協会東北大会プログラムおよび講演予稿集   Vol. 2014   page: 72   2014.9

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    J-GLOBAL

  20. 走査型イオンコンダクタンス顕微鏡を用いた単一細胞ナノバイオプシー技術の開発と細胞内mRNA局在性の評価

    梨本裕司, 高橋康史, 伊野浩介, 井上(安田)久美, 珠玖仁, 末永智一

    日本分析化学会年会講演要旨集   Vol. 63rd   page: 26   2014.9

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    J-GLOBAL

  21. 界面イオン伝導顕微鏡による正極薄膜材料表面におけるLiイオン挿入・脱離機構の可視化

    熊谷明哉, 高橋康史, 猪又宏貴, 白木将, 山本邦子, 春田正和, 伊野浩介, 珠玖仁, 一杉太郎, 末永智一

    応用物理学会秋季学術講演会講演予稿集(CD-ROM)   Vol. 75th   page: ROMBUNNO.19A-A8-1   2014.9

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    J-GLOBAL

  22. マイクロガラスピペットによるmicroRNA回収・分析法

    宮下紘介, 梨本裕司, 高橋康史, 伊野浩介, 珠玖仁, 末永智一

    化学とマイクロ・ナノシステム学会研究会講演要旨集   Vol. 29th   page: 78   2014.5

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    J-GLOBAL

  23. 微小ガラスプローブを用いたヒト培養細胞のmicroRNA回収および定量

    宮下紘介, 梨本裕司, 高橋康史, 伊野浩介, 珠玖仁, 末永智一

    分析化学討論会講演要旨集   Vol. 74th   page: 36   2014.5

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    J-GLOBAL

  24. DEVELOPMENT OF LIQUID-JUNCTION-FREE SUBSTITUTIONAL STRIPPING DEVICE FOR HIGHLY SENSITIVE BIOSENSING

    Proceedings of the Chemical Sensor Symposium   Vol. 56   page: 10 - 12   2014.3

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  25. Development of Carbon Nano-Heater: Stimulation of Sensory Neurons for Functional Study of Heat Sensitive Channels (vol 104, pg 519a, 2013)

    Babak Babakinejad, Takahashi Yasufumi, Takahashi Yasufumi, Yuri Korchev, Paolo Actis

    BIOPHYSICAL JOURNAL   Vol. 104 ( 8 ) page: 1834 - 1834   2013.4

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    DOI: 10.1016/j.bpj.2013.03.006

    Web of Science

  26. Quantitative Characterization of Local Chemical Delivery through Nanopipette

    Babak Babakinejad, Takahashi Yasufumi, Peter Joensson, Pavel Novak, Andriy Shevchuk, Uma Anand, David Klenerman, Yuri Korchev

    BIOPHYSICAL JOURNAL   Vol. 102 ( 3 ) page: 313A - 313A   2012.1

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    Language:English   Publishing type:Research paper, summary (international conference)   Publisher:CELL PRESS  

    Web of Science

  27. 走査型電気化学/イオンコンダクタンス顕微鏡を用いた生体試料の高解像度イメージング

    末永 智一, 高橋 康史, 伊野 浩介, 珠玖 仁, KORCHEV Y. E., MACPHERSON J. V., UNWIN P. R., KLENERMAN D.

    ポーラログラフィー   Vol. 57 ( 3 ) page: 232 - 232   2011.11

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    CiNii Books

  28. Development of ultra-multipoint electrochemical detection systems

    Proceedings of the Chemical Sensor Symposium   Vol. 47   page: 109 - 111   2009.3

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  29. 走査型イオンコンダクタンス顕微鏡を用いた細胞膜表面観察と局所電気浸透流インジェクションへの応用

    高橋康史, 村上有美, 安川智之, 珠玖仁, 神崎展, 末永智一

    電気化学会大会講演要旨集   Vol. 75th   page: 435   2008.3

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    J-GLOBAL

  30. 複合酵素による走査型電気化学顕微鏡の電流シグナルの増幅と細胞膜タンパク質検出への応用

    高橋康史, 宮本健史, 安川智之, 珠玖仁, 浅野竜太郎, 熊谷泉, 末永智一

    分析化学討論会講演要旨集   Vol. 69th   2008

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  31. 単一細胞由来mRNA回収マイクロプローブの開発

    珠玖仁, 梨本裕司, 高橋康史, 安川智之, 阿部宏之, 末永智一

    日本化学会講演予稿集   Vol. 87th ( 2 )   2007

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  32. 高感度ナノ電気化学顕微鏡を用いた細胞膜タンパク質のイメージング

    高橋康史, 宮本健史, 安川智之, 珠玖仁, 浅野竜太郎, 熊谷泉, 末永智一

    応用物理学会学術講演会講演予稿集   Vol. 68th ( 3 )   2007

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  33. 多機能ナノ電気化学顕微鏡を用いた単一生細胞表面の膜タンパク質局所イメージング

    高橋康史, 宮本健史, 安川智之, 珠玖仁, 浅野竜太郎, 熊谷泉, 末永智一

    電気化学秋季大会講演要旨集   Vol. 2007   2007

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  34. シアフォース電気化学/近接場光顕微鏡によるリアルタイム生体イメージング

    高橋康史, 平野悠, 安川智之, 珠玖仁, 末永智一

    電気化学会大会講演要旨集   Vol. 73rd   2006

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  35. シアフォース電気化学・近接場光学顕微鏡の開発とバイオイメージングへの応用

    高橋康史, 平野悠, 安川智之, 珠玖仁, 末永智一

    化学とマイクロ・ナノシステム研究会講演要旨集   Vol. 13th   2006

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Presentations 172

  1. 走査型プローブ顕微鏡を用いた生細胞の動的イメージング Invited

    髙橋康史

    JST CREST 統合1細胞解析のための革新的技術基盤 非標識神経伝達物質イメージセンサによる細胞活動可視化システム構築と脳機能の時空間解析 2020 CREST 合同ミーティング in 中伊豆  2020.1.30 

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    Event date: 2020.1

    Language:Japanese   Presentation type:Public lecture, seminar, tutorial, course, or other speech  

  2. Nanoscale Electrochemical Imaging using Scanning Probe Microscopy Invited

    Yasufumi Takahashi

    1st WPI NanoLSI-iCeMS Joint Symposium on Nanoimaging and Advanced Materials for Life Science  2020.1.23 

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    Event date: 2020.1

    Language:English   Presentation type:Symposium, workshop panel (nominated)  

  3. Visualization of Inhomogeneous Reactivity Using Scanning Electrochemical Cell Microscopy Invited

    Yasufumi Takahashi

    Electrochemistry Gordon Research Conference  2020.1.10 

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    Event date: 2020.1

    Language:English   Presentation type:Oral presentation (invited, special)  

  4. Live cell functional imaging using scanning probe microscopy Invited International conference

    TAKAHASHI Yasufumi

    3rd NanoLSI Symposium at UBC in Vancouver  2019.8.8 

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  5. ナノ電気化学セル顕微鏡を用いたグラフェン/グラファイト表面構造における電気化学活性の評価

    三浦千穂, 熊谷明哉, 岡田健, 寒川誠二, 寒川誠二, 珠玖仁, 高橋康史, 高橋康史, 末永智一

    応用物理学会秋季学術講演会講演予稿集(CD-ROM)  2017.8.25 

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  6. ナノ電気化学セル顕微鏡を用いたグラファイト/グラフェン表面の電気化学活性の可視化

    熊谷明哉, 高橋康史, 三浦千穂, 珠玖仁, 末永智一, 末永智一

    電気化学会大会講演要旨集(CD-ROM)  2016.3.23 

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  7. Catalytic Active Site Imaging of MoS2 Nanosheet by using nanoSECCM

    TAKAHASHI Yasufumi

    2016.3.29 

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    File: takahashi1.pdf

  8. ナノ電気化学セル顕微鏡を用いた 局所的な電気化学計測 Invited

    高橋 康史

    平成28年度資源・素材関係学協会合同秋季大会  2016.9.13 

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  9. Observation of Hydrogen Storage Reaction Distribution for BCC-Type alloy Surface Using nano-Scanning Electrochemical Cell Microscopy (nanoSECCM)

    田中元基, 熊谷明哉, 近真紀雄, 陶山博司, 西山博史, 中西真二, 珠玖仁, 高橋康史, 高橋康史, 射場英紀, 末永智一

    電池討論会講演要旨集  2017.11.13 

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  10. ナノ電気化学セル顕微鏡の局所電気化学測定を利用したSEI被膜生成過程の解析

    渡邊徹弥, 熊谷明哉, 阿部真知子, 岡崎智子, 伊藤友一, 佐藤悠人, 井田大貴, 珠玖仁, 高橋康史, 高橋康史, 射場英紀, 末永智一

    電池討論会講演要旨集  2016.11.28 

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  11. ナノ電気化学セル顕微鏡による中和型ポリアクリル酸バインダーを用いたSi‐黒鉛複合負極の特性評価

    渡邊徹弥, 熊谷明哉, 高橋康史, 山際清史, 久保田圭, 井田大貴, 珠玖仁, 駒場慎一, 末永智一, 末永智一

    電気化学会大会講演要旨集(CD-ROM)  2016.3.23 

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  12. ナノ電気化学セル顕微鏡によるグラフェン/グラファイト構造における電気化学活性の局所電気化学測定と可視化

    三浦千穂, 熊谷明哉, 岡田健, 寒川誠二, 寒川誠二, 珠玖仁, 高橋康史, 高橋康史, 末永智一, 末永智一

    応用物理学会春季学術講演会講演予稿集(CD-ROM)  2017.3.1 

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  13. ナノ電気化学セル顕微鏡によるSi‐黒鉛複合電極用架橋型ポリアクリル酸バインダーの有機電解液の分解抑制効果の検証

    JUNG S, 佐藤悠人, 熊谷明哉, 高橋康史, 高橋康史, 久保田圭, 瀧本一樹, 水田浩徳, 岡本訓明, 珠玖仁, 駒場慎一, 末永智一

    応用物理学会秋季学術講演会講演予稿集(CD-ROM)  2017.8.25 

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  14. ナノ電気化学セル顕微鏡によるSi‐黒鉛複合負極の局所電気化学特性評価

    渡邊徹弥, 熊谷明哉, 高橋康史, 高橋康史, 久保田圭, 井田大貴, 珠玖仁, 駒場慎一, 末永智一

    電池討論会講演要旨集  2016.11.28 

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  15. ナノ電気化学セル顕微鏡によるSi‐C複合電極用架橋型ポリアクリル酸バインダーの局所電気化学評価

    熊谷明哉, 佐藤悠人, 高橋康史, 高橋康史, 久保田圭, 瀧本一樹, 水田浩徳, 岡本訓明, 珠玖仁, 駒場慎一, 末永智一, 末永智一

    電気化学会大会講演要旨集(CD-ROM)  2017.3.17 

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  16. ナノ電極・ナノピペットを用いた電気化学イメージング技術を用いた単一細胞計測

    高橋康史

    第12回 生体界面研究会  2020.2.17 

  17. ナノプローブを用いた1細胞mRNAの局所回収及び発現量解析

    周縁殊, 梨本裕司, 高橋康史, 高橋康史, 福間剛士, 珠玖仁, 末永智一, 末永智一

    日本分析化学会年会講演要旨集  2016.8.31 

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  18. ナノスケールの神経細胞の形状イメージングを 実現する走査型イオンコンダクタンス顕微鏡の開発

    高橋 康史

    第77回分析化学討論会  2017.5.27 

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  19. Development of Nano Electrochemical Microcopy for Visualizing Nanoscale Reaction on Solid-Liquid Interface Invited

    TAKAHASHI Yasufumi

    2016.3.30 

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    File: takahashi 受賞講演3.pdf

  20. シナプスの形状変化を捉える走査型イオンコンダクタンス顕微鏡の開発

    Yasufumi Takahashi, Takafumi Miyamoto, Zhou Yuanshu, Takeshi Fukuma

    第84回電気化学会大会  2017.3.27 

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  21. ケミカルマッピングを実現する ナノ電気化学顕微鏡の創成

    高橋 康史

    日本化学会第98回春季大会(2018)コラボレイション企画 JST さきがけ「統合1細胞解析のための革新的技術基盤」領域-1期生(平成26年度採択)- 第2回研究成果報告会:革新的なバイオイメージングと1細胞解析技術開発  2018.3.22 

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  22. グラフェンエッジにおける電気化学活性のナノスケール電気化学イメージング

    熊谷明哉, 熊谷明哉, 三浦千穂, 高橋康史, 高橋康史, 井田大貴, 珠玖仁, 末永智一

    日本分析化学会年会講演要旨集  2018.8.29 

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  23. グラファイト/グラフェンのエッジ領域における電気化学活性の可視化

    熊谷明哉, 高橋康史, 三浦千穂, 珠玖仁, 末永智一, 末永智一

    応用物理学会春季学術講演会講演予稿集(CD-ROM)  2016.3.3 

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  24. エンドサイトーシスを直接可視化する 走査型イオンコンダクタンス顕微鏡の開発

    高橋 康史, 宮本 貴史, 井田 大貴, 東 宏樹, 周 縁殊, 福間 剛士

    【応用物理学会】2019春季講演会  2019.3.12 

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  25. Visualization of Nanoscale Inhomogeneous Current Distribution on ZrO2-Coated LiCoO2 Thin-Film Electrodes using SECCM Invited International conference

    TAKAHASHI Yasufumi

    9th Workshop on Scanning Electrochemical Microscopy (SECM)  2017.8.15 

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  26. Visualization of Nanoscale Inhomogeneous Current Distribution on ZrO2-Coated LiCoO2 Thin-Film Electrodes using SECCM Invited International conference

    TAKAHASHI Yasufumi

    2018.9.13 

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  27. SnS<sub>2</sub>二次元薄膜における水素発生反応のナノスケール電気化学イメージング

    小川寛人, 熊谷明哉, 熊谷明哉, 上野啓司, 井田大貴, 高橋康史, 末永智一, 珠玖仁

    日本分析化学会年会講演要旨集  2018.8.29 

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  28. Single cell analysis using scanning probe microscopy Invited International conference

    TAKAHASHI Yasufumi

    Single cell biology meets diagnostics workshop  2019.3.4 

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  29. SECM‐SICMを用いた酵素反応検出

    中村拓生, 伊野浩介, 梨本裕司, 梨本裕司, 熊谷明哉, 高橋康史, 高橋康史, 末永智一, 珠玖仁

    日本分析化学会年会講演要旨集  2018.8.29 

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  30. Nanoscale Live Cell Chemical and Topographical Imaging using Scanning Probe microscopy Invited International conference

    高橋 康史

    MPFI-JST workshop  2018.10.30 

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  31. Nanoscale imaging of extracellular microenvironment using scanning ion conductance microscopy Invited

    TAKAHASHI Yasufumi

    2019.3.15 

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  32. Nanoscale Electrochemical Reactivity Imaging on Boron-Doped Diamond Using Scanning Electrochemical Cell Microscopy Invited International conference

    Yasufumi Takahashi, Tomohiro Ando, Kai Asai, Yuanshu Zhou, Yasuaki Einaga, Takeshi Fukuma

    International Symposium on Diamond Electrochemistry (Final Symposium of JST-ACCEL project “Fundamentals and Applications of Diamond Electrodes”)  2019.3.6 

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  33. Nanoscale electrochemical imaging by scanning probe microscopy Invited International conference

    高橋 康史

    International Workshop: New Electroanalytical Techniques and Their Emerging Applications (IWNET-2017)  2017.9.26 

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  34. Multifunctional Scanning Ion Conductance Microscopy for Single Cell Analysis Invited International conference

    高橋 康史

    Meeting of the German Society for Biochemistry and Molecular Biology  2017.9.23 

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  35. Live Cell Nanoscale Topography and Chemical Imaging by Using Scanning Ion Conductance Microscopy and Scanning Electrochemical Microscopy Invited

    TAKAHASHI Yasufumi

    23rd iCeMS International Symposium “Emerging Science for Unlocking Cell's Secrets”  2017.5.30 

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  36. Live Cell Imaging using Scanning Probe Microscopy Invited

    TAKAHASHI Yasufumi

    2016.7.28 

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  37. ナノ電気化学セル顕微鏡を用いたグラフェンの電気化学応答評価

    三浦千穂, 熊谷明哉, 熊谷明哉, 岡田健, 寒川誠二, 寒川誠二, 珠玖仁, 高橋康史, 高橋康史, 末永智一

    電気化学会東北支部セミコンファレンス講演論文集  2017 

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  38. 電気化学計測が可能な⾛査型プローブ顕微鏡を⽤いた機能性イメージング Invited

    高橋康史

    セミナー(慶應義塾大学先端生命科学研究所)  2019.12.11 

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  39. 電気化学界面・デバイスの 局所評価技術の基礎と応用 Invited

    高橋 康史

    【応用物理学会】2019春季講演会  2019.3.9 

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  40. 電気化学イメージングによる金属/半導体カーボンナノチューブの酸化還元反応の検証

    志村実優, 熊谷明哉, 熊谷明哉, 岡田健, 三浦千穂, 井田大貴, 寒川誠二, 寒川誠二, 珠玖仁, 高橋康史, 高橋康史, 末永智一

    電気化学会大会講演要旨集(CD-ROM)  2018.2.23 

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  41. 金属/半導体単層カーボンナノチューブのナノ電気化学イメージング

    志村実優, 熊谷明哉, 熊谷明哉, 岡田健, 三浦千穂, 寒川誠二, 寒川誠二, 珠玖仁, 高橋康史, 高橋康史, 末永智一

    電気化学会東北支部セミコンファレンス講演論文集  2017 

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  42. 酸化還元反応の差異による半導体・金属カーボンナノチューブの検出

    熊谷明哉, 熊谷明哉, 志村実優, 高橋康史, 高橋康史, 三浦千穂, 岡田健, 岡田健, 井田大貴, 珠玖仁, 寒川誠二, 寒川誠二, 末永智一

    応用物理学会春季学術講演会講演予稿集(CD-ROM)  2018.3.5 

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  43. 遷移金属ダイカルコゲナイドナノシートの触媒活性イメージング

    高橋 康史, 太田 真登, 小林 佑, 熊谷 明哉, 宮田 耕充, 福間 剛士

    【応用物理学会】2019春季講演会  2019.3.12 

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  44. 超高解像度電気化学顕微鏡の創成と応用

    青柳重夫, 松岡涼, 高橋康史, 珠玖仁, 末永智一

    ポーラログラフィーおよび電気分析化学討論会講演要旨集(Web)  2017 

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  45. 超解像度ケミカルイメージング 技術の開発 Invited

    高橋 康史

    第2回フロンティアバイオイメージング研究会  2017.11.7 

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  46. 走査型電気化学セル顕微鏡を用いたカルコゲナイド系層状物質の電気化学イメージング

    太田真登, 山下翼, 小林佑, 宮田耕充, ZHOU Yuanshu, 福間剛士, 高橋康史, 高橋康史

    電気化学会大会講演要旨集(CD-ROM)  2018.2.23 

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  47. 走査型電気化学セル顕微鏡を使用した単結晶ダイヤモンドの電気化学イメージング

    安藤智洋, 浅井開, 栄長泰明, ZHOU Yuanshu, ZHOU Yuanshu, 福間剛士, 福間剛士, 高橋康史, 高橋康史

    電気化学秋季大会講演要旨集(CD‐ROM)  2018.9.11 

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  48. 走査型電気化学セル顕微鏡によるリチウム電池電極の局所的な拡散係数の計測

    山下翼, 高松大郊, ZHOU Yuanshu, ZHOU Yuanshu, 福間剛士, 福間剛士, 高橋康史, 高橋康史

    電気化学秋季大会講演要旨集(CD‐ROM)  2018.9.11 

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  49. 走査型電気化学セル顕微鏡によるLi<sub>4</sub>Ti<sub>5</sub>O<sub>12</sub>の充放電特性イメージング

    山下翼, 高松大郊, ZHOU Yuashu, 福間剛士, 高橋康史, 高橋康史

    電気化学会大会講演要旨集(CD-ROM)  2018.2.23 

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  50. Chemical concentration profile imaging using scanning electrochemical microscopy and scanning ion conductance microscopy hybrid system Invited

    Takahashi Yasufumi, Ida Hiroki, Zhou Yuanshu, Shiku Hitoshi, Matsue Tomokazu

    2016.3.9 

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    File: 学会4.pdf

  51. 走査型プローブ顕微鏡を用いた局所電気化学計測 Invited

    高橋 康史

    2017年 電気化学会北陸支部秋季大会プログラム  2017.11.2 

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  52. 走査型プローブ顕微鏡を用いたコモンスペにおけるケミカルセシグ

    高橋 康史

    第10回生体界面研究会  2019.2.28 

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  53. 走査型プローブ顕微鏡を用いた 生細胞の動的イメージング Invited

    高橋康史

    セミナー(産業技術総合研究所)  2019.12.6 

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  54. 走査型プローブ顕微鏡を用いた 単一細胞の電気化学イメージング Invited

    高橋 康史

    第92回日本生化学会  2019.9.18 

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  55. 走査型プローブ顕微鏡を用いた ライブセル超解像度イメージング Invited

    高橋 康史

    2018年電気化学秋季大会  2018.9.25 

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  56. 走査型プローブ顕微鏡を利用した電気化学計測 Invited

    高橋 康史

    環境微生物系合同大会  2017.8.29 

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  57. 走査型プローブ顕微鏡による細胞表面でのケミカルセンシング Invited

    高橋康史, 井田大貴, 周縁殊, 藤井拓人, 酒井秀紀, 珠玖仁, 福間剛士

    第95回日本生理学会大会  2018.3.29 

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  58. 走査型プローブ顕微鏡によるエンドサイトーシスの直接可視化

    高橋康史, 東宏樹, 井田大貴, 周縁殊, 福間剛士

    第71回細胞生物学会  2019.6.25 

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  59. 走査型プローブ顕微鏡による1次繊毛の非標識イメージング Invited

    高橋 康史

    第92回日本薬理学会年会  2019.3.14 

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  60. 走査型プローブ顕微鏡による 生細胞の超解像度ケミカルイメージング Invited

    高橋 康史

    日本物理学会第73回年次大会  2018.3.24 

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  61. 走査型プローブ顕微鏡とイオン伝導計測技術の融合によるイオン伝導パスの可視化技術の創成

    高橋康史

    旭硝子財団研究助成成果発表会  2017.7 

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  62. 走査型イオンコンダクタンス顕微鏡を用いた負極材料の形状とイオン濃度プロファイルの可視化

    高橋 康史, 高松 大効, 周 縁殊, 福間 剛士

    2019年 電気化学秋季大会  2019.9.6 

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  63. 走査型イオンコンダクタンス顕微鏡を用いた神経細胞のナノスケールイメージング

    高橋 康史, 宮本貴史, 周縁殊, 福間剛士

    日本生物物理学会第55回年会  2017.9.19 

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  64. 走査型イオンコンダクタンス顕微鏡を用いたリチウムイオン二次電池電極表面の形状観察

    小笠原航汰, 熊谷明哉, 高橋康史, 猪又宏貴, 井田大貴, 高松大郊, 山際清史, 久保田圭, 珠玖仁, 駒場慎一, 末永智一, 末永智一

    電気化学会大会講演要旨集(CD-ROM)  2016.3.23 

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  65. 走査型イオンコンダクタンス顕微鏡を用いたエンドサイトーシスの観察

    宮本貴史, ZHOU Yuanshu, ZHOU Yuanshu, 東宏樹, 福間剛士, 福間剛士, 高橋康史, 高橋康史

    電気化学秋季大会講演要旨集(CD‐ROM)  2018.9.11 

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  66. 走査型イオンコンダクタンス顕微鏡によるタンパク質薄膜表面の電荷評価

    今井俊輔, LI Fei, YANG Peng, 井田大貴, 熊谷明哉, 高橋康史, 高橋康史, 伊野浩介, 珠玖仁, 末永智一

    化学とマイクロ・ナノシステム学会研究会講演要旨集  2017.10.4 

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  67. 走査型イオンコンダクタンス顕微鏡によるタンパク質薄膜表面のナノスケール電荷マッピング

    今井俊輔, LI Fei, YANG Peng, 井田大貴, 熊谷明哉, 熊谷明哉, 高橋康史, 高橋康史, 伊野浩介, 珠玖仁, 末永智一

    電気化学会大会講演要旨集(CD-ROM)  2018.2.23 

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  68. 走査型イオンコンダクタンス顕微鏡によるタンパク質薄膜の電荷マッピング

    今井俊輔, LI Fei, YANG Peng, 井田大貴, 熊谷明哉, 熊谷明哉, 高橋康史, 高橋康史, 伊野浩介, 珠玖仁, 末永智一

    電気化学会東北支部セミコンファレンス講演論文集  2017 

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  69. 走査型イオンコンダクタンス顕微鏡(SICM)を用いた細胞表面上エクソソーム計測

    東宏樹, 吉田孟史, 吉田孟史, ZHOU Yuanshu, ZHOU Yuanshu, 宮本貴史, 華山力成, 華山力成, 福間剛士, 福間剛士, 高橋康史, 高橋康史

    電気化学秋季大会講演要旨集(CD‐ROM)  2018.9.11 

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  70. 薄膜シールド機構を備えた液中AFMの開発

    宮澤佳甫, 山村俊貴, 泉久範, 高橋康史, 高橋康史, 福間剛士, 福間剛士

    応用物理学会秋季学術講演会講演予稿集(CD-ROM)  2017.8.25 

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  71. 細胞観察用の延伸AFM探針の開発と性能評価

    日笠山拓, 宮澤佳甫, ZHOU Yuanshu, 高橋康史, 高橋康史, 高橋康史, 福間剛士, 福間剛士

    応用物理学会春季学術講演会講演予稿集(CD-ROM)  2018.3.5 

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  72. Development of scanning ion conductance microscopy for time-lapse imaging of neuron

    Yasufumi Takahashi, Takafumi Miyamoto, Zhou Yuanshu, Takeshi Fukuma

    日本化学会 第97春季年会 (2017)  2017.3.17 

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  73. Development of Scanning Electrochemical - Ion Conductance Microscopy for Single Cell Analysis International conference

    高橋 康史

    NUS-JST (PRESTO) Workshop  2016.12.9 

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  74. Development of Nano Electrochemical Microscopy for Chemical Mapping Invited

    高橋 康史

    日本化学会第96春季年会  2016.3.25 

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    File: sample_Word_english4.pdf

  75. Development of Nano Electrochemical Microcopy for Single Cell Analysis Invited

    高橋 康史

    日本分析化学会第65年会  2016.9.14 

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  76. Development of multifunction scanning ion conductance microscopy for single cell analysis International conference

    高橋 康史

    4th Kanazawa Bio-AFM Workshop  2016.10.5 

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  77. Development of High Resolution Scanning Electrochemical Microscopy for Single Cell Analysis Invited International conference

    高橋 康史

    Pittcon 2017  2017.3.8 

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  78. Super resolution live cell functional imaging Invited

    TAKAHASHI Yasufumi

    2019.9.26 

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  79. Development of Scanning Ion Conductance Microscopy for Non-label Biophysiological Interphase Chemical Imaging Invited

    Takahashi Yasufumi, Zhou Yuanshu, Ida Hiroki, Shiku Hitoshi, Sakai Hideki, Matsue Tomokazu

    2016.3.23 

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    File: 抄録登録 [10044].eml

  80. 水素貯蔵合金表面におけるナノ電気化学イメージング

    安永幹生, 熊谷明哉, 熊谷明哉, 田中元基, 高橋康史, 高橋康史, 末永智一, 珠玖仁

    日本分析化学会年会講演要旨集  2018.8.29 

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  81. 水素/空気二次電池用水素吸蔵合金における電気化学応答の可視化

    田中元基, 熊谷明哉, 近真起雄, 陶山博司, 西山博史, 中西真二, 珠玖仁, 高橋康史, 高橋康史, 射場英紀, 末永智一, 末永智一

    電気化学会大会講演要旨集(CD-ROM)  2017.3.17 

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  82. ライブセルの超解像度形状イメージング技術と代謝物の電気化学計測技術の開発 Invited

    高橋康史

    第80回分析化学討論会  2020.5.23 

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  83. マイクロ電極を用いた電気化学測定の実際

    青柳重夫, 松岡涼, 松平昌昭, 高橋康史, 熊谷明哉, 珠玖仁, 末永智一

    日本分析化学会年会講演要旨集  2017.8.26 

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  84. ナノ電気化学顕微鏡を用いたBCC系合金における水素貯蔵過程の可視化

    熊谷明哉, 田中元基, 近真紀雄, 陶山博司, 西山博史, 中西真二, 珠玖仁, 高橋康史, 高橋康史, 射場英紀, 末永智一

    応用物理学会秋季学術講演会講演予稿集(CD-ROM)  2017.8.25 

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  85. ナノ電気化学セル顕微鏡を用いたリチウムイオン電池Si‐黒鉛複合負極の評価

    熊谷明哉, 渡邊徹弥, 高橋康史, 高橋康史, 久保田圭, 佐藤悠人, 珠玖仁, 駒場慎一, 末永智一, 末永智一

    応用物理学会春季学術講演会講演予稿集(CD-ROM)  2017.3.1 

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  86. 非標識・非侵襲でのナノスケールの形状観察を実現する 走査型イオンコンダクタンス顕微鏡の開発と応用 Invited

    高橋 康史

    第69回日本細胞生物学会大会  2017.6.13 

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  87. ケミカルマッピングを実現する ナノ電気化学顕微鏡の創成 Invited

    高橋 康史

    日本化学会第96春季年会  2016.3.27 

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    File: 日本語4.pdf

  88. 高解像度電気化学イオンコンダクタンス顕微鏡によるアルミダイガストの腐食特性の検証

    青柳重夫, 松岡涼, 松本尚志, 松平昌昭, 高橋康史, 高橋康史, 熊谷明哉, 井田大貴, 棟方裕一, 珠玖仁, 金村聖志, 末永智一

    電気化学会大会講演要旨集(CD-ROM)  2017.3.17 

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  89. Direct visualization of nanoscale inhomogeneous reactivity of lithium-ion battery using SECCM Invited

    Yasufumi Takahashi

    2021.12.19 

  90. ナノピペットを利用したナノスケールの電気化学イメージング技術の開発と応用 Invited

    高橋康史

    日本表面真空学会学術講演会  2021.11.3 

  91. ガラスナノピペットを用いた細胞のナノ構造・機能解明に資するプローブ顕微鏡の開発 Invited

    高橋康史

    第167委員会第98回研究会  2021.7.29 

  92. ガラスナノピペットを用いた単一オルガネラの単離と分析 Invited

    高橋康史

    第44回日本分子生物学会年会  2021.12.3 

  93. Nanoscale electrochemical reactivity imaging on BDD using scanning electrochemical cell microscopy Invited

    Yasufumi Takahashi

    2021.6.7 

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  94. Nanoscale electrochemical imaging for Visualizing the Heterogeneous Catalytic Activity Invited

    Yasufumi Takahashi

    2021.8.13 

  95. Labviewを使った走査型プローブ顕微鏡用プログラムの開発と応用 Invited

    高橋康史

    第81回分析化学討論会  2021.5.22 

  96. Electrochemical mapping of hydrogen evolution reaction site on transition metal dichalcogenide nanosheets Invited

    Yasufumi Takahashi

    2021.12.21 

  97. Development of Voltage Switching Mode Scanning Electrochemical Microscopy for Topographical and Electrochemical Nanoscale Imaging of Living Cells International conference

    Yasufumi Takahashi, Andrew I. Shevchuk, Pavel Novak, Yoshiharu Matsumae, Babak Babakinejad, Julie V. Macpherson, Patrick R. Unwin, Kosuke Ino, Hitoshi Shiku, Julia Gorelik, David Klenerman, Yuri E. Korchev, Tomokazu Matsue

    222nd Meeting of Electrochemical Society  2012.10.8 

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  98. Development of Voltage Switching Mode Scanning Electrochemical Microscopy for Nanoscale Electrochemical Imaging Invited International conference

    Yasufumi Takahashi, Yoshiharu Matsumae, Kosuke Ino, Hitoshi Shiku, Yuri E. Korchev, Tomokazu Matsue

    5. 14th Topical Meeting of the International Society of Electrochemistry  2014.3.30 

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  99. Development of Nanoscale Meniscus Cell Microscope for Visualizing Li+ (de)intercalation Dynamics at LiFePO4 Cathodes International conference

    Yasufumi Takahashi, Akichika Kumatani, Hirokazu Munakata, Hirotaka Inomata, Hitoshi Shiku, Patrick R. Unwin, Yuri E. Korchev, Kiyoshi Kanamura, Tomokazu Matsue

    65th Annual Meeting of the International Society of Electrochemistry  2014.9.1 

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  100. Development of High Resolution Scanning Electrochemical Microscopy for Nanoscale Topographical and Electrochemical Imaging of Living Cells International conference

    Yasufumi Takahashi, Hitoshi Shiku, Patrick R. Unwin, Yuri E. Korchev, Tomokazu Matsue

    65th Annual Meeting of the International Society of Electrochemistry  2014.9.1 

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  101. Development of a Novel Combined Scanning Electrochemical Microscope (SECM) and Scanning Ion-Conductance Microscope (SICM) Probe for Soft Sample Imaging International conference

    Andrew J. Pollard, Nilofar Faruqui, Michael Shaw, Charles A. Clifford, Yasufumi Takahashi, Yuri E. Korchev, Neil Ebejer, Julie V. Macpherson, Patrick R. Unwin, Debdulal Roy

    2011.11.28 

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  102. Characterize Cell Function using SECMSICM International conference

    Yasufumi Takahashi, Yoshiharu Matsumae, Hitoshi Shiku, Kosuke Ino, Yuri Korchev, Tomokazu Matsue

    221st Meeting of Electrochemical Society  2012.5.8 

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    Language:English   Presentation type:Oral presentation (general)  

  103. Electrochemical and Topographical Imaging of Living Cell using SECM-SICM International conference

    Yasufumi Takahashi, Kosuke Ino, Hitoshi Shiku, Tomokazu Matsue

    3rd Kanazawa Bio-AFM Workshop  2012.11.5 

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  104. 高速走査型イオンコンダクタンス顕微鏡による細胞表面構造の非侵襲定量追跡

    井田大貴, 高橋康史, 高橋康史, 熊谷明哉, 珠玖仁, 末永智一, 末永智一

    応用物理学会春季学術講演会講演予稿集(CD-ROM)  2016.3.3 

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  105. 高解像度走査型イオンコンダクタンス顕微鏡の開発

    青柳重夫, 松岡涼, 松平昌昭, 高橋康史, 末永智一

    Rev Polarogr  2015.10.27 

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  106. 走査型電気化学・走査型イオンコンダクタンス顕微鏡を用いた生体イメージング Invited

    高橋 康史

    公益社団法人日本顕微鏡学会第57回シンポジウム  2013.11.16 

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  107. 細胞表面構造の定量的な動態評価を可能にする高速走査型イオンコンダクタンス顕微鏡

    井田大貴, 高橋康史, 高橋康史, 熊谷明哉, 珠玖仁, 末永智一, 末永智一

    日本細胞生物学会大会(Web)  2016 

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  108. 生細胞のナノスケールでの形状イメージングを実現する 走査型イオンコンダクタンス顕微鏡の開発 Invited

    髙橋 康史

    自然科学研究機構プロジェクト 合同シンポジウム 「脳神経情報の階層的研究」 「機能生命科学における揺らぎと決定」  2015.3.11 

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  109. 局所的な電気化学計測を実現するナノ電気化学顕微鏡の開発

    高橋康史, 高橋康史, 高橋康史, 熊谷明哉, 珠玖仁, 末永智一, 末永智一

    日本分析化学会年会講演要旨集  2015.8.26 

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  110. 中和型ポリアクリル酸塩バインダーを用いたSi/C複合電極の局所特性評価

    渡邊徹弥, 熊谷明哉, 高橋康史, 山際清史, 久保田圭, 井田大貴, 珠玖仁, 駒場慎一, 末永智一, 末永智一

    電気化学会東北支部セミコンファレンス講演論文集  2015.12.4 

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  111. レドックスサイクルに基づく神経伝達物質の検出に向けた新規CMOS型デバイスの開発

    阿部博弥, 伊野浩介, LI Chen‐Zhong, LI Chen‐Zhong, 菅野佑介, 井上(安田, 久美, 國方亮太, 須田篤史, 松平昌昭, 高橋康史, 高橋康史, 珠玖仁, 末永智一, 末永智一

    化学とマイクロ・ナノシステム学会研究会講演要旨集  2015.11.26 

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  112. リチウム酸化物薄膜電極の作製とナノ電気化学セル顕微鏡による電池特性評価

    熊谷明哉, 高橋康史, 白木将, 春田正和, 猪又宏貴, 渡邊徹弥, 井田大貴, 珠玖仁, 一杉太郎, 末永智一, 末永智一

    電気化学会東北支部セミコンファレンス講演論文集  2015.12.4 

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  113. ナノ電気化学顕微鏡を用いたケミカルマッピング Invited

    髙橋 康史

    化学系学協会東北大会  2014.9.21 

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  114. ナノ電気化学セル顕微鏡を用いたリチウムイオン二次電池材料の局所充放電特性マッピング

    高橋康史, 熊谷明哉, 猪又宏貴, 棟方裕一, 伊野浩介, 珠玖仁, 金村聖志, 末永智一

    日本化学会講演予稿集  2015.3.11 

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  115. ナノ電気化学セル顕微鏡を用いたLiCoO<sub>2</sub>薄膜表面の局所電気化学測定

    熊谷明哉, 高橋康史, 高橋康史, 高橋康史, 清水亮太, 渡邊徹弥, 猪又宏貴, 白木将, 珠玖仁, 一杉太郎, 末永智一, 末永智一

    応用物理学会秋季学術講演会講演予稿集(CD-ROM)  2015.8.31 

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  116. ナノ電気化学セル顕微鏡を用いたLiCoO<sub>2</sub>薄膜表面におけるZrO<sub>2</sub>被覆効果の検討

    猪又宏貴, 熊谷明哉, 高橋康史, 高松大郊, 伊野浩介, 珠玖仁, 末永智一

    電気化学会大会講演要旨集(CD-ROM)  2015.3.9 

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  117. ナノ電気化学セル顕微鏡を用いたLiCoO<sub>2</sub>薄膜へのZrO<sub>2</sub>被覆効果に関する考察

    猪又宏貴, 熊谷明哉, 高橋康史, 高橋康史, 高橋康史, 高松大郊, 珠玖仁, 末永智一, 末永智一

    電池討論会講演要旨集  2015.11.10 

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  118. ナノ電気化学セル顕微鏡によるLi過剰Mn層状酸化物電極表面の電流応答の可視化

    小笠原航汰, 高橋康史, 熊谷明哉, 山際清史, 久保田圭, 井田大貴, 珠玖仁, 駒場慎一, 末永智一, 末永智一

    電気化学会東北支部セミコンファレンス講演論文集  2015.12.4 

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  119. ナノ電極・ナノピペットを利用した走査型プローブ顕微鏡の新展開 Invited

    高橋 康史

    JSPSナノプローブテクノロジー第167委員会 「第76回研究会」  2014.10.23 

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  120. ナノ電極・ナノピペットを利用した生体界面での局所計測

    高橋康史, 珠玖仁, 伊野浩介, 井上久美, Yuri Korchev, 末永智一

    第2 回生体界面研究  2015.2.20 

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  121. ナノ電極・ナノピペットを利用したナノ界面計測 Invited

    高橋 康史

    金沢大学バイオAFM先端研究センターセミナー  2015.5.13 

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  122. グラフェン/グラファイト表面構造における電気化学応答の可視化

    三浦千穂, 熊谷明哉, 高橋康史, 井田大貴, 珠玖仁, 末永智一

    電気化学会東北支部セミコンファレンス講演論文集  2016 

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  123. ガラスピペット内における細胞塊の培養とエクソソームの検出

    宮下紘介, 井田大貴, 梨本裕司, ZHOU Yuanshu, 伊野浩介, 高橋康史, 珠玖仁, 末永智一, 末永智一

    電気化学秋季大会講演要旨集(CD‐ROM)  2015.9.7 

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  124. Simultaneous Noncontact Topography and Electrochemical Nanoscale Imaging by using Scanning Probe Microscope Invited

    TAKAHASHI Yasufumi

    2014.1.8 

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  125. SICM による細胞表面のタイムラプスイメージングと局所遺伝子回収への応用

    高橋 康史

    第4 回生体界面研究会  2016.2.2 

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  126. Nanoscale Imaging of Living Cells using Nano-Scanning Electrochemical Microscopy International conference

    TAKAHASHI Yasufumi

    10th International Conference on Fuild Dynamics  2013.11.25 

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  127. Development of Nano Scanning Electrochemical Cell Microscopy for Visualizing Charge/discharge Property of LiFePO4 Cathodes Invited International conference

    TAKAHASHI Yasufumi

    8th SECM workshop  2015.10.10 

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    File: SECM8_abstract-template3.doc

  128. Development of Nano Electrochemical Microscopy for Chemical and Biological Imaging

    TAKAHASHI Yasufumi

    2015.3.23 

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  129. Close型バイポーラー電極システムを用いた液絡不要の変換ストリッピングボルタンメトリ法の検討

    井上久美, 高野真一朗, 池川未歩, 高橋康史, 伊野浩介, 珠玖仁, 末永智一

    Rev Polarogr  2015.10.27 

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  130. Topography Imaging of Hippocampus Spine using Scanning Ion Conductance Microscopy International conference

    Yasufumi Takahashi, Kosuke Ino, Hitoshi Shiku, Tomokazu Matsue

    XXIII International Symposium on Morphological Sciences  2013.9.20 

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  131. Topographical and Electrochemical Nanoscale Imaging of Living Cells using Nano-Scanning Electrochemical Microscopy Invited International conference

    Yasufumi Takahashi

    7. The Fourteenth International Symposium on Electroanalytical Chemistry  2013.8.20 

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  132. Scanning Electrochemical Ion-conductance Hybrid Microscopy for Nanoscale Chemical Imaging of Live International conference

    Yasufumi Takahashi, Andrew I. Shevchuk, Pavel Novak, Yuri E. Korchev

    UK SPM meeting  2011.6.22 

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  133. Lithium-Ion Transport at Electrolyte/Electrode Interface Visualized By Nanoscale Meniscus Cell Microscope International conference

    Akichika Kumatani, Yasufumi Takahashi, Hirotaka Inomata, Hirokazu Munakata, Kosuke Ino, Hitoshi Shiku, Kiyoshi Kanamura, Tomokazu Matsue

    226th Meeting of Electrochemical Society  2014.10.6 

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  134. In-situ characterization and mapping of lithium-ion transport at the electrolyte/cathode interface by high resolution ion-conductance microscopy International conference

    Akichika Kumatani, Yasufumi Takahashi, Hirokazu Munakata, Hirotaka Inomata, Kosuke Ino, Hitoshi Shiku, Kiyoshi Kanamura, Tomokazu Matsue

    E-MRS 2013 FALL MEETING  2013.9.18 

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  135. Improving the Electrochemical Measurement Sensitivity of SECM-SICM by using Pt Electrodeposited Carbon Nanoelectrode International conference

    Yasufumi Takahashi, Sen Mustafa, Hiroki Ida, Hitoshi Shiku, Tomokazu Matsue

    66th Annual Meeting of the International Society of Electrochemistry  2015.10.7 

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    File: ABSTRACTS_TEMPLATE.doc

  136. Improving the electrochemical Imaging sensitivity of SECM-SICM by using size adjustable Pt electrodeposited carbon nanoelectrode International conference

    TAKAHASHI Yasufumi

    Pacifichem 2015  2015.12.18 

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    File: abstract.pdf

  137. High-resolution bioelectrochemical imaging with SECM-SICM hybrid system International conference

    Yasufumi Takahashi, Kosuke Ino, Hitoshi Shiku, Tomokazu Matsue

    International Association of Colloid and Interface Scientists Conference 2012  2012.5.12 

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  138. Evaluation of Differentiation State of an Embryonic Stem Cell Using Scanning Electrochemical Microscopy International conference

    Yasufumi Takahashi, Yoshiharu Matsumae, Kosuke Ino, Hitoshi Shiku, Tomokazu Matsue

    223rd Meeting of Electrochemical Society  2013.5.13 

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  139. 化学・ナノ構造カップリングの解明に資する対話型分析技術の創成

    高橋康史

    2022年度北川パネル進捗会議  2022.10.17 

  140. ナノ電極・ナノピペットを用いた電気化学イメージング技術の新展開 Invited

    高橋康史

    2022電気化学秋季大会  2022.9.11 

  141. ナノピペットを用いた細胞膜表面の超解像度イメージング Invited

    高橋康史

    コロイド先端技術講座2021  2022.2.8 

  142. ナノピペットを用いたライブセルイメージング・センシング Invited

    高橋康史

    基盤医学特論 異分野融合推進セミナー 第2回  2022.11.28 

  143. ナノスケールの電気化学イメージング技術の創成

    さきがけ 「電子やイオン等の能動的制御と反応」領域 オンライン公開シンポジウム  2022.1.8 

  144. ナノスケールの細胞機能評価を実現する走査型プローブ顕微鏡 Invited

    高橋康史

    第37回マルチモーダルバイオイメージセンサ研究会  2022.12.13 

  145. ガラスナノピペットを用いた機能性イメージング技術の創成 Invited

    高橋康史

    表面界面スペクトロスコピー2022  2022.12.9 

  146. ガラスナノピペットを用いたバイオイメージング Invited

    高橋康史

    生体内情報計測・バイオイメージングのための 先端メディカルデバイス開発の最前線  2023.2.27 

  147. ガラスナノピペットを利用した 新奇プローブ顕微鏡の開発と応用 Invited

    高橋康史

    FRIS/TI-FRIS Material Science Seminar 2022  2022.7.19 

  148. Visualization of the catalytic activity on 2 D materials using scanning probe microscopy Invited

    高橋康史

    第64回フラーレン・ナノチューブ・グラフェン総合シンポジウム  2023.3.3 

  149. Super-resolution chemical imaging using scanning probe microscopy Invited

    高橋康史

    Bioinspired Engineering and Biomechanics Center (BEBC) of Xi'an Jiaotong University seminar  2022.12.21 

  150. Development of Organelle Collection Technology Using Nanopipette Invited

    高橋康史

    6th NanoLSI Symposium  2022.11.14 

  151. 2.5次元材料における局所触媒活性の実空間イメージング

    高橋康史

    学術変⾰領域研究(A)「2.5次元物質科学︓社会変⾰に向けた物質科学のパラダイムシフト」 第3回 領域会議  2022.10.15 

  152. 単一オルガネラ分析に資する走査型プローブ顕微鏡の開発 Invited

    高橋康史

    第31回日本バイオイメージング学会  2022.9.4 

  153. 走査型電気化学セル顕微鏡を用いたオペランド電気化学イメージング 技術の開発と応用 Invited

    キャラクタリゼーション講習会  2022.1.11 

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  154. 走査型プローブ顕微鏡による 超解像度ライブセルイメージング Invited

    高橋康史

    九州大学理学研究院化学部門 分析化学特別講演会  2022.7.7 

  155. 走査型イオンコンダクタンス顕微鏡を用いた 単一オルガネラ回収技術の開発 Invited

    高橋康史

    第45回日本分子生物学会年会  2022.11.30 

  156. 触媒活性の実空間イメージング技術の創成 Invited

    高橋康史

    開拓プロジェクト最終シンポジウム  2022.3.4 

  157. 触媒活性の実空間イメージングに資するプローブ顕微鏡の開発 Invited

    高橋康史

    [ナノプローブテクノロジー167委員会]第101回研究会  2022.3.3 

  158. 細胞の表面をナノスケールで 観察する顕微鏡の開発と応用 Invited

    高橋康史

    GTR-ITbM-RCMS Seminar  2022.4.20 

  159. 生細胞表面の超解像度形状イメージング技術の開発 Invited

    高橋康史

    ITbM/GTRコンソーシアムワークショップ  2022.6.29 

  160. 激しく変化する社会において学生に求められる能力

    名古屋大学拠点博士過程学生交流セミナー2022 

  161. 機械学習を利用した細胞の自動回収技術の開発

    高橋康史

    細胞の局所コミュニティ研究会  2022.12.20 

  162. 2.5次元材料における局所触媒活性の 実空間イメージング

    高橋康史

    学術変革領域研究(A)「2.5次元物質科学:社会変革に向けた物質科学のパラダイムシフト」 第4回 領域会議  2023.3.13 

  163. 2.5次元材料における局所触媒活性の 実空間イメージング

    高橋康史

    学術変革領域研究(A)「2.5次元物質科学:社会変革に向けた物質科学のパラダイムシフト」 第5回 領域会議  2023.7.1 

  164. 2.5次元材料における局所触媒活性の 実空間イメージング

    高橋康史

    学術変革領域研究(A)「2.5次元物質科学:社会変革に向けた物質科学のパラダイムシフト」 第6回 領域会議  2023.12.26 

  165. 細胞の自動回収を実現するナノピペット技術の開発 Invited

    高橋康史

    第83回分析化学討論会  2023.5.20 

  166. 水素発生をはじめとする触媒活性を可視化する 電気化学イメージング Invited

    高橋康史

    二次元材料に関する koine meeting  2024.1.19 

  167. 微小電極・ナノピペットを用いた 単一細胞計測 Invited

    高橋康史

    第97回日本薬理学会  2023.12.14 

  168. 単一オルガネラ操作に資する 走査型イオンコンダクタンス顕微鏡の開発 Invited

    高橋 康史

    第96回日本生化学会大会  2023.11.1 

  169. ガラスナノピペットを用いたオルガネラのその場回収技術の開発 Invited

    高橋康史

    第75回日本細胞生物学会  2023.6.28 

  170. ガラスナノピペットを用いた 機能性イメージング技術の創成 Invited

    高橋康史

    第3回マテリアル・計測ハイブリッド研究センター シンポジウム  2023.7.5 

  171. ガラスナノピペットを用いた オペランドイメージング Invited

    高橋康史

    第119回新電池構想部会  2023.4.19 

  172. オルガネラレベルの分析を実現する 走査型イオンコンダクタンス顕微鏡の開発

    高橋康史

    第2回GTPハッカソン  2023.12.10 

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KAKENHI (Grants-in-Aid for Scientific Research) 18

  1. Metal tolerance and metal adsorption through phycosphere control

    Grant number:23H02303  2023.4 - 2027.3

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research  Grant-in-Aid for Scientific Research (B)

  2. ナノ空間を巧みに利用した革新的ナノポアケミカルセンサーの創成

    Grant number:22K18939  2022.6 - 2025.3

    日本学術振興会  科学研究費助成事業 挑戦的研究(萌芽)  挑戦的研究(萌芽)

    高橋 康史

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    Authorship:Principal investigator 

    Grant amount:\6500000 ( Direct Cost: \5000000 、 Indirect Cost:\1500000 )

    細胞内でオルガネラは相互作用しながら活動しており、その理解には、細胞内の化学動態を計測する技術がもとめられている。そこで、ガラスピペットに酵素やアプタマーを修飾し、化学物質の濃度をセンサー薄膜の電荷状態の変化としてとらえる。さらに、能動的に生体分子をナノポア内に導入する手法、導入した生体分子の増幅法を確立し、細胞の代謝物をセンシング可能な革新的なケミカルセンサーを確立する。

  3. 生体膜ナノ構造の可視化と脂質網羅分析のための統合ナノ分析システム

    Grant number:22K18950  2022.6 - 2024.3

    日本学術振興会  科学研究費助成事業 挑戦的研究(萌芽)  挑戦的研究(萌芽)

    川井 隆之, 高橋 康史

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    生体膜の局所的ナノ構造を可視化し,構成する分子組成を明らかにするための「統合ナノ分析システム」を世界で初めて実現し,生体膜ナノ構造に基づく未知の生命原理や疾患の分子機序を明らかにするための技術基盤を構築する。生細胞膜のナノ構造を可視化できる走査型イオン伝導顕微鏡でナノドメインを捕捉して採取し,ナノキャピラリー電気泳動-質量分析で解析する統合ナノ分析システムを開発する。これにより,ナノドメインの時空間情報と脂質分子組成などの化学情報の両面から生体膜の実態解明を目指す。

  4. 2.5次元材料における局所触媒活性の実空間イメージング

    Grant number:22H05459  2022.6 - 2024.3

    日本学術振興会  科学研究費助成事業 学術変革領域研究(A)  学術変革領域研究(A)

    高橋 康史

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    Authorship:Principal investigator 

    Grant amount:\6760000 ( Direct Cost: \5200000 、 Indirect Cost:\1560000 )

    2次元材料の触媒活性向上に向けて、モアレ、歪、欠陥、ドーピング、ヘテロジャンクションの形成など様々な試みがなされてきた。このような構造を巧みに利用した触媒開発において、触媒能と構造の関係性の理解は喫緊の課題である。本研究では、電気化学イメージング技術である走査型電気化学セル顕微鏡(SECCM)を用いて2.5次元材料の触媒活性サイトを、実空間で電気化学的に可視化する。

  5. 化学・ナノ構造カップリングの解明に資する対話型分析技術の創成

    2022 - 2028

    科学技術振興機構  戦略的な研究開発の推進 創発的研究支援事業 

    高橋 康史

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    バイオロジーの発展に新しい計測・イメージング技術の開発が不可ですが、オルガネラレベルや、組織深部の分析・操作技術が欠けています。そこで、これまで培ってきたナノピペットによる分子レベルの刺激技術や、生細胞イメージングのノウハウを活用し、細胞と対話するようにセンシングと刺激を印加できる新しい技術の走査型プローブ顕微鏡技術の開発し、化学・ナノ構造カップリングによる新たなバイオロジーの世界を開拓します。

  6. がん細胞の表現型と遺伝子発現状態をひもとく次世代イオンコンダクタンス顕微鏡の創成

    Grant number:21H01770  2021.4 - 2025.3

    日本学術振興会  科学研究費助成事業 基盤研究(B)  基盤研究(B)

    Korchev Yuri.E., ZHANG YANJUN, 高橋 康史, 周 縁殊

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    Authorship:Coinvestigator(s) 

    SICM のピペット先端にセンサーを搭載し、形状とともにpHe、ROS 産生能、硬さなどの表現型を単一細胞レベルでイメージングした。その後、同一のピペットで細胞質を回収し、遺伝子発現評価を行った。pHe やROS 産生能は、癌細胞の代謝状態やミトコンドリア活性と関連し、癌の増殖と密接に関わっている。そこで、SICM のナノピペットに、グルコースオキシダーゼとポリL リシンの混合液を充填し、グルタルアルデヒドで架橋し、薄膜状のpH 感受性の膜をナノピペットの先端に有するpH プローブを独自開発した。また、ナノピペット内にカーボン電極を形成し、その表面にPt を電着させることで、電気化学的な細胞内のROS 計測も実証済みである。癌細胞の硬さは、細胞骨格と密接に関係しており、浸潤や転移のしやすさを示すバイオマーカーである。SICM では、イオン電流を利用しているため、細胞にほぼダメージを与えずに、高感度に硬さの違いを計測できる。 遺伝子発現評価に関しては、これまでの手法は細胞を破砕するため、時々刻々と変化する細胞内の遺伝子発現状態を知ることは困難であった。SICMナノピペットを用いた細胞質のサンプリングでは、微小量の細胞質を複数回回収できるため、同一の細胞のmRNAの局在や動態を評価できる。

  7. Understanding and controls of reaction intermediates in electrochemical carbon dioxide reduction and development of gaseous flow type electrolytic synthesis cell

    Grant number:21H02037  2021.4 - 2025.3

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research Grant-in-Aid for Scientific Research (B)  Grant-in-Aid for Scientific Research (B)

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    Authorship:Coinvestigator(s) 

  8. Measurement of battery material interface from electrophysiological viewpoint

    Grant number:20K21141  2020.7 - 2022.3

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research Grant-in-Aid for Challenging Research (Exploratory)  Grant-in-Aid for Challenging Research (Exploratory)

    Takahashi Yasufumi

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    Authorship:Principal investigator 

    Grant amount:\6500000 ( Direct Cost: \5000000 、 Indirect Cost:\1500000 )

    Scanning ion-conductance microscopy (SICM) uses a glass pipette as a probe for imaging live cell surface topography using ion current feedback control. In this study, we modified SICM for evaluating the ion concentration profile change during the charge / discharge of the hard carbon anode. As a result, we have established an analytical technique that contributes to an understanding of SEI and presentation of design guidelines, such as the search for the optimum additive for desolvation during high-speed charging and discharging.

  9. Development of new scanning probe microscopy for correlative analysis of nanoscale structure change and signal transduction

    Grant number:20H02582  2020.4 - 2023.3

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research Grant-in-Aid for Scientific Research (B)  Grant-in-Aid for Scientific Research (B)

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    Authorship:Principal investigator 

    Grant amount:\17810000 ( Direct Cost: \13700000 、 Indirect Cost:\4110000 )

  10. Collective cell migration by activation wave of growth factor signal transduction cascade

    Grant number:19H00993  2019.4 - 2024.3

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research Grant-in-Aid for Scientific Research (A)  Grant-in-Aid for Scientific Research (A)

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    Authorship:Coinvestigator(s) 

  11. Water Oxidation on Semiconductor Photocatalysts: How Completed under Dilute Photon Flux

    Grant number:19H00915  2019.4 - 2022.3

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research Grant-in-Aid for Scientific Research (A)  Grant-in-Aid for Scientific Research (A)

    ONISHI HIROSHI

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    Authorship:Coinvestigator(s) 

    Researchers in Japan have developed semiconductor photocatalysts highly efficient for the overall water splitting reaction to produce H2 and O2. Why are they active? This is the fundamental question that drives this three-year research project. We developed two methods for characterization of photocatalysts working under water. Time-resolved detection of O2 released into water was achieved with platinum microelectrode. Infrared light absorption of photocatalyst particles irradiated with ultraviolet light for excitation was monitored on a diamond prism. The developed methods were successfully applied to NaTaO3 and SrTiO3 photocatalysts.

  12. Sodium Tantalate (NaTaO3) Photocatalysts: Why So Active for Water Splitting

    Grant number:16H02250  2016.4 - 2019.3

    Grants-in-Aid for Scientific Research  Grant-in-Aid for Scientific Research (A)

    ONISHI HIROSHI, Hanggara Sudrajat, An Longjie, Zhou Yizhong, Ogura Takuya, Fujiwara Tomoya, Sato Takamasa, Teduka Yuya, Kosaka Takumu, Ichikuni Nobuyuki, Sasahara Akira, Wöll Christof, Babel Snadhya

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    Authorship:Coinvestigator(s) 

    Sodium tantalate (NaTaO3) is the first semiconductor photocatalyst which produces hydrogen-oxygen mixed bubbles in the overall water splitting reaction, when properly doped with metal cations. This research project has been organized to answer the question of why doping with metal cations raised the quantum efficiency of the reaction. In-depth studies focused on Sr cation doping revealed that the electron-hole recombination rate was reduced when Ta cations were exchanged with Sr cations. Sodium cations were simultaneously exchanged to balance the cationic and anionic charges to form NaTaO3-Sr(Sr1/3Ta2/3)O3 solid solution. In addition, the intra-particle distribution of Sr cations played an essential role. Strontium cations segregated to produce graded composition from the Sr-rich surface to the Sr-poor core. The bottom of the conduction band lifted up at the Sr-rich surface, and the excited electrons were driven to the Sr-poor core leaving holes at the surface.

  13. ナノ電気化学セル顕微鏡による界面反応計測

    Grant number:16H00885  2016.4 - 2018.3

    日本学術振興会  科学研究費助成事業 新学術領域研究(研究領域提案型)  新学術領域研究(研究領域提案型)

    高橋 康史

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    Authorship:Principal investigator 

    Grant amount:\5980000 ( Direct Cost: \4600000 、 Indirect Cost:\1380000 )

    畜電池の高速充放電の実現には、電池材料の反応メカニズムの詳細な理解が求められている。放射光技術によるオペランド計測がこのような充放電過程における準安定構造の存在を証明したが、これらの影響と電池特性を結びつけるには、通常の電気化学計測法では時空間分解が課題である。これまで開発してきたナノ電気化学セル顕微鏡(NanoSECCM)は、ナノピペットを利用して電池構造をナノ空間で再現し、イオンの挿入脱離に伴う電流を測定する。本手法を用いて、これまで得ることのできなかった高速充放電中に生じる固/液界面、固/固界面での変化を理解する。本年度は、サイクル特性向上のために、コバルト酸リチウム(LCO)表面に形成したZrO2の酸化物層の被覆形態と電気化学特性の関係をSECCMにより評価した。LCO薄膜電池上に、ZrO2の酸化物層をパルスレーザーデポジション法(PLD)により形成した。ZrO2の厚みは、PLDの成膜時間により調整した。未被覆、30秒被覆、180秒ZrO2をそれぞれ製膜したでLCO薄膜電池に関して、SECCMイメージングを行った。レート特性とサイクル特性に優れたZrO2の30秒被覆の試料において、電気化学イメージングを行うと、未被覆と180秒被覆では見られなかった島状の不均一な電流イメージを得ることができた。これは、ZrO2の厚さに不均一性があり、島状に電流応答の低い部分が見られたと考えられる。このZrO2が厚い領域では、LCO表面をZrO2がしっかり保護することでサイクル特性を良好に保つことができたと考えられる。一方、ZrO2の薄い部分が存在することで、レート特性をある程度維持できていたものと考えられる。このようにこれまで可視化することができなかった酸化物層による電池表面の不均一性をSECCMにより可視化することに成功した。

  14. Development of interface ion conductance microscopy

    Grant number:15H05422  2015.4 - 2019.3

    Grants-in-Aid for Scientific Research  Grant-in-Aid for Young Scientists (A)

    Takahashi Yasufumi

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    Authorship:Principal investigator 

    Grant amount:\23790000 ( Direct Cost: \18300000 、 Indirect Cost:\5490000 )

    In order to fill the gap between the theoretical and the actual capacity of the storage battery, it is necessary to visualize the reactivity on battery material surface as an electrochemical operando imaging. To visualize inhomogeneous reactivity on battery material, we have developed scanning electrochemistry cell microscope (SECCM). SECCM uses electrolyte solution filled nanopipette to form a nanoscale electrochemical cell between nanopipette and sample to characterize the local electrochemical reactivity. In this work, we improved the SECCM software for CV imaging or charge/discharge imaging, established controlled SECCM which place in grove box for evaluating the negative electrode material, and elucidated the metal oxide modification effect of the cathode material surface.

  15. Ion conductance imaging using litium based probe microscopy

    Grant number:15K13263  2015.4 - 2017.3

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research Grant-in-Aid for Challenging Exploratory Research  Grant-in-Aid for Challenging Exploratory Research

    TAKAHASHI YASUFUMI

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    Authorship:Principal investigator 

    Grant amount:\4030000 ( Direct Cost: \3100000 、 Indirect Cost:\930000 )

    In this study, we developed new scanning probe microscopy for electrochemical imaging of the cathode/solid electrolyte interface resistance.The new microscope is based on the positioning technology using electrochemical signals, principle of high-speed, high-sensitivity electrochemical measurement of nanoscale electrochemical measurement, and low noise electrochemical system. We developed the electrochemical imaging system that can measure not only in the atmospheric environment but also inside the glove box. We also developed solid electrolyte probes and electron conductivity / ion conductivity simultaneous imaging probes and improved the resolution of imaging.

  16. Innovative electrochemical imaging device for bioanalysis

    Grant number:25248032  2013.5 - 2016.3

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research Grant-in-Aid for Scientific Research (A)  Grant-in-Aid for Scientific Research (A)

    Matsue Tomokazu, INO KOSUKE, TAKAHASHI YASUFUMI, RAMON JAVIER, SHIKU HITOSHI, INOUE KUMI

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    Authorship:Coinvestigator(s) 

    In the present study, we have developed two-types of electrochemical devices for bioimaging. One was a bio-LSI device which was based on large-scale integrated (LSI) circuits dedicated to bioanalysis. The other was a local redox cycling-based electrochemical (LRC-EC) device utilizing local redox cycling. The device consisted of many switching sensors incorporated into a small chip device to detect electrochemical responses. These bioimaging devices were successfully applied for evaluation of oxygen consumption and secreted chemicals from cells, and cell differentiation.

  17. Real-time monitoring of chemical transport on cell membrane using nano-SECM

    Grant number:24710140  2012.4 - 2014.3

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research Grant-in-Aid for Young Scientists (B)  Grant-in-Aid for Young Scientists (B)

    TAKAHASHI YASUFUMI

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    Authorship:Principal investigator 

    Grant amount:\4940000 ( Direct Cost: \3800000 、 Indirect Cost:\1140000 )

    Chemical transport on the cell membrane is important issue for developement of drug delivery system and improvement of gene transfection. In this study, the dynamic cell surface fluctuation was detected or visualised by using nano electrode. The electrochemical measurement is effective for evaluation of mass transfer on liquid/solid interface. I developed fabrication method of nanoelectrode and nanopositioning system for quantitative analysis and time-lapse imaging of mass transfer on cell membrane.

  18. 多機能ナノ電気化学顕微鏡を用いた膜タンパク質の機能解析と細胞操作への応用

    Grant number:08J04808  2008 - 2009

    日本学術振興会  科学研究費助成事業 特別研究員奨励費  特別研究員奨励費

    高橋 康史

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    膜タンパク質の発現状態は疾病と密接な関わりがあり、遺伝子あるいは環境の影響を特定するため、その場での観察可能な分析技術が求められる。そこで、細胞の活性・代謝を電気的に評価可能な走査型電気化学顕微鏡(SECM)をベースとし、プローブであるマイクロ電極に加工を施し、形状・電気化学・光学測定を同時に行う多機能ナノ電気化学顕微鏡を開発した。
    本システムは、細胞をディッシュから剥離せずに膜タンパク質を評価可能なため、細胞剥離時に生じる膜タンパク質へのダメージの影響を受けない。また、異種類の細胞パターンの同時評価が可能である。発現状態が癌の増殖・分化と密接な関わりがある上皮成長因子受容体(EGFR)について、異種類の細胞について膜タンパク質の発現量評価に成功し、これまでの報告と高い相関性が見られた。
    電気化学測定は細胞表面のセンシングに有効であり、光学測定と組み合わせることで、細胞の内外を明瞭に識別できる。そこで、光ファイバー電極を用いて、GFPの遺伝子と放出型アルカリフォスファターゼ(SEAP)を共発現させたHeLa細胞の測定を行った。HeLa細胞の細胞内に発現したGFPに起因した蛍光と、細胞外に放出されたSEAPの酵素活性に起因した酸化電流を光ファイバー電極により同時に検出することができた。さらに、シアフォース距離制御を行うことで細胞の形状測定と、電気化学測定および蛍光測定の高感度化に成功した。
    接着性の細胞は、細胞-細胞間の相互作用によりmRNAの発現状態が変化するため、選択的かつ迅速な回収技術が求められる。そこで、`中空リング電極を用いて、局所的にパルス電位(40V,10μs)を印加し、単一細胞を破砕・回収し、定量的遺伝子評価(リアルタイムPCR)を行った。基板接着に関与するインテグリンの遺伝子について、単一細胞での遺伝子発現量の定量に成功し、電場破砕による遺伝子への影響がないことを証明した。

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Industrial property rights 7

  1. リアクタ

    平井 健二, 高橋 康史

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    Applicant:国立大学法人北海道大学

    Application no:特願2021-007115  Date applied:2021.1

    Announcement no:特開2021-178311  Date announced:2021.11

    J-GLOBAL

  2. 成膜装置一体型顕微鏡

    高橋 康史, 鯉沼 秀臣, 佐藤 利弘, 松木 伸行

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    Applicant:国立大学法人金沢大学

    Application no:特願2020-093058  Date applied:2020.5

    Announcement no:特開2021-188987  Date announced:2021.12

    J-GLOBAL

  3. 走査型プローブ顕微鏡及びその制御方法

    高▼橋 康史

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    Applicant:国立大学法人金沢大学

    Application no:特願2016-188803  Date applied:2016.9

    Announcement no:特開2018-054385  Date announced:2018.4

    J-GLOBAL

  4. 走査型電気化学イオンコンダクタンス顕微鏡、その探針及び探針の製造方法。

    高橋 康史, 末永 智一, 珠玖 仁, 村上 有美, 長峯 邦明, アンドリュー・シェヴチャク, ユーリ・コルチェフ

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    Applicant:国立大学法人東北大学, インペリアル イノベーションズ リミテッド

    Application no:特願2009-140602  Date applied:2009.6

    Announcement no:特開2010-261923  Date announced:2010.11

    Patent/Registration no:特許第5467473号  Date issued:2014.2

    J-GLOBAL

  5. 走査型電気化学イオンコンダクタンス顕微鏡測定法、走査型電気化学イオンコンダクタンス顕微鏡、その探針および探針の製造方法

    高橋 康史, 末永 智一, 珠玖 仁, 村上 有美, 長峯 邦明, アンドリュー・シェヴチャク, ユーリ・コルチェフ

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    Applicant:国立大学法人東北大学, インペリアル イノベーションズ リミテッド

    Application no:特願2009-140602  Date applied:2009.6

    Announcement no:特開2010-261923  Date announced:2010.11

    J-GLOBAL

  6. 電気化学測定装置

    末永 智一, 林 振宇, 高橋 康史, 梅村 太三, 北川 雄介, 安川 智之, 國方 亮太, 珠玖 仁

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    Applicant:国立大学法人東北大学

    Application no:特願2008-175120  Date applied:2008.7

    Announcement no:特開2010-014558  Date announced:2010.1

    Patent/Registration no:特許第5176235号  Date issued:2013.1

    J-GLOBAL

  7. 電気化学測定装置

    末永 智一, 林 振宇, 高橋 康史, 梅村 太三, 北川 雄介, 安川 智之, 國方 亮太, 珠玖 仁

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    Applicant:国立大学法人東北大学

    Application no:特願2008-175120  Date applied:2008.7

    Announcement no:特開2010-014558  Date announced:2010.1

    J-GLOBAL

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Media Coverage 7

  1. ナノ構造光電極の電荷分離機構を実空間で可視化 ~太陽光水分解の材料開発を促進~ Internet

    Acs Catal 2022, 12 (2), 1201-1208.  2022.1

  2. 探針型の顕微鏡でチップ内の血管機能を可視化 ~生体模倣システムの新たな計測法を開発~ Internet

    Adv Healthc Mater 2021, e2101186.  2021.8

  3. 生きた細胞膜での膜透過性ペプチドの取り込みをナノスケールで可視化 細胞膜で起こる様々な物質のやり取りや反応を直接観察可能に Internet

    Anal. Chem., 2021, 93 (13), 5383-5393.  2021.3

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    Acs Catal 2021, 11 (6), 3310-3318.  2021.3

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