研究者詳細 - 萩尾　健史

論文 - 萩尾　健史

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Utilization of agricultural waste to herbicide removal: Magnetic BEA zeolite adsorbents prepared by dry-gel conversion using rice husk ash-derived SiO2 for paraquat removal 査読有り国際共著国際誌

Phouthavong Vanpaseuth, Hagio Takeshi, Park Jae-Hyeok, Nijpanich Supinya, Srihirunthanon Teeranun, Chantanurak Nutchanan, Duangkhai Kanchanok, Rujiravanit Ratana, Chounlamany Vanseng, Phomkeona Kesiny, Kong Long, Li Liang, Ichino Ryoichi

ARABIAN JOURNAL OF CHEMISTRY 16 巻 ( 8 ) 2023年8月

担当区分：責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Arabian Journal of Chemistry

This study presents a method that will allow for the sustainable utilization of rice husk ash-SiO2 (RHAS), an agricultural-waste–derived material, as a bulky solid SiO2 source in the zeolite beta (BEA)/Fe3O4 composite (magnetic RHAS-BEA) synthesis via a dry-gel conversion method for the removal of paraquat, a typical herbicide, from aqueous solutions. Ultrasonic waves were used to facilitate the formation of uniform Fe3O4-contained dry precursor gel before converting to the magnetic BEA zeolite composite for the first time. Magnetic RHAS-BEA was then characterized and compared with a non-magnetic sample (RHAS-BEA) using X-ray diffraction and field-emission scanning electron microscopy. In terms of adsorption, we found that paraquat had a high adsorption rate on the samples and conformed to a pseudo-second-order kinetic model. The adsorption behavior of paraquat on the synthesized RHAS-BEA and magnetic RHAS-BEA obeyed the Langmuir adsorption isotherm model. The synthesized adsorbents were reusable for at least four cycles, via thermal regeneration at 450 °C. The inclusion of Fe3O4 particles in magnetic RHAS-BEA disrupted neither the crystallization of the BEA zeolite nor the adsorption of paraquat and enabled easy collection via an external magnet.

DOI： 10.1016/j.arabjc.2023.104959

Dry-gel conversion synthesis of magnetic BEA-type zeolites for antibiotics adsorption 査読有り国際共著国際誌

Phouthavong Vanpaseuth, Hagio Takeshi, Nijpanich Supinya, Park Jae-Hyeok, Hiraiwa Masatake, Srihirunthanon Teeranun, Chantanurak Nutchanan, Rujiravanit Ratana, Kamimoto Yuki, Li Xinling, Kong Long, Li Liang, Ichino Ryoichi

JOURNAL OF SOL-GEL SCIENCE AND TECHNOLOGY 105 巻 ( 2 ) 頁： 511 - 524 2023年2月

担当区分：責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Journal of Sol-Gel Science and Technology

The dry-gel conversion method (DGC) is a promising synthesis protocol for preparing magnetic zeolite composites as it yields homogeneous composite particles with more rapid crystallization, smaller reactor volume, and less waste production than the conventional hydrothermal method. This work investigates the optimal conditions for preparing magnetic BEA-type zeolites using the DGC method, including the gel/water ratio, crystallization temperature and time. Precursor dry-gel incorporating well-dispersed magnetite was subjected to crystallization under water vapor atmosphere with a gel/water ratio of 0.5–2, crystallization temperature of 140–200 °C for 1.5–12 h, followed by characterization using X-ray diffraction and scanning electron microscopy. The optimum conditions were found to be gel/water ratio of 1 and crystallization at 180 °C for 12 h. Magnetic properties of collected samples were evaluated using a vibrating-sample magnetometer after calcination at 400–500 °C for 12 h. Products calcined below 450 °C showed good magnetic properties. Adsorption of sulfadiazine using the BEA and magnetic BEA-type zeolites was evaluated in a 10–50 mg/l range. Results revealed favorable multilayer-type adsorption of sulfadiazine onto both non-magnetic and magnetic BEA-type zeolites (Freundlich model). These indicate that DGC method is suitable for preparing high-silica magnetic BEA-type zeolites with potential for antibiotic removal. Graphical Abstract: [Figure not available: see fulltext.].

DOI： 10.1007/s10971-022-06025-2

Electrodeposition of Amorphous Molybdenum Oxide on Iron-Group Element Based Plating and its Novel Application as a Corrosion Protective Coating 査読有り国際共著国際誌

Park Jae-Hyeok, Hagio Takeshi, Nijpanich Supinya, Chanlek Narong, Chaiprapa Jitrin, Songsiriritthigul Chomphunuch, Songsiriritthigul Prayoon, Ichino Ryoichi

JOURNAL OF THE ELECTROCHEMICAL SOCIETY 169 巻 ( 7 ) 2022年7月

担当区分：責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Journal of the Electrochemical Society

The corrosion resistance of materials composed of metal is an essential property for preventing material deterioration caused by corrosion. In this study, we demonstrate that corrosion resistance can be significantly improved through the electrodeposition of molybdenum oxide onto a metal plating containing iron-group elements. Mo oxide can be electrodeposited using a simple plating bath, low current density, and short deposition time, exhibiting a fascinating metallic gloss appearance. GI-XRD and XPS analyses revealed that amorphous Mo oxide adhered to the substrate by a seed layer partially reduced to metallic Mo by the iron-group element in the substrate, based on the principle of "induced co-deposition."A Mo oxide coating with a thickness of approximately 100 nm decreases the corrosion current density of Ni-W plating by approximately 5 times and the passivation current density by approximately 10 times in a 3 mass% NaCl solution. Mo oxide coatings represent an attractive strategy for improving the corrosion resistance of various metal materials containing iron-group elements.

DOI： 10.1149/1945-7111/ac7e78

A tri-layer floating photocatalyst/adsorbent for the removal of organic compounds from wastewater: Layer-by-layer deposition of silicalite-1 and titania on hollow glass microspheres 査読有り国際共著国際誌

Environmental Technology and Innovation 26 巻 2022年5月

担当区分：責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Environmental Technology and Innovation

Removal of organic compounds from wastewater is necessary to ensure that aquatic organisms are not adversely affected. In the past, it had been shown that zeolite-based systems provide good opportunities for wastewater treatment; however, most of the zeolite systems reported thus far face the disadvantages of sinking in water and saturated adsorption site. Therefore, in the current study, we attempted to develop zeolite-based composite systems with good floatability, adsorption capacity, and photocatalytic activity. In addition, our aim was to ensure that these composites could be easily separated from the treated water. Thus, a tri-layer floating photocatalyst/adsorbent was prepared via the layer-by-layer deposition of silicalite-1, a pure silica MFI-type zeolite (PSZ), and TiO2 on hollow glass microspheres (HGMs). A thin layer of silicalite-1 was crystallized on the dense walls of HGMs to fabricate floating adsorbents (PSZ-HGMs). Subsequently, a layer of TiO2 was deposited on PSZ-HGM surfaces using the sol–gel method to develop photocatalytic composites (TiO2/PSZ-HGMs). A good PSZ coverage and attachment were achieved on HGM surfaces by adding HGMs to an alkali solution containing tetrapropylammonium hydroxide and tetraethyl orthosilicate, followed by hydrothermal synthesis at 180 °C for 40 h. Subsequent deposition of TiO2 was effective in homogeneously covering the PSZ surface without clogging the zeolite pores. The wastewater treatment capacity of the synthesized materials was verified using methylene blue (MB). It was found that TiO2/PSZ-HGMs, which exhibited both photocatalytic and adsorption activities, acted synergistically with UV-C irradiation to drastically degrade MB concentration by ∼98% within 2 h. Therefore, these materials may be considered to have high potential in wastewater-treatment processes.

DOI： 10.1016/j.eti.2021.102242

Development of novel nanoporous hexagonal tungsten oxide membrane for separation of water/acetic acid mixtures via pervaporation 査読有り国際誌

Kunishi Hiroto, Hagio Takeshi, Wada Shintaro, Kamimoto Yuki, Ichino Ryoichi

JOURNAL OF MEMBRANE SCIENCE 620 巻 2021年2月

担当区分：責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Journal of Membrane Science

A novel nanoporous hexagonal tungsten oxide (NP-h-WO3) membrane was developed for separating water/acetic acid (H2O/AcOH) mixtures. The nanopores on the c-plane of h-WO3 are larger than H2O molecules and smaller than AcOH molecules and thus should allow for their effective separation. Moreover, h-WO3 exhibits high stability in acids (pH < 4). Therefore, c-axis-aligned NP-h-WO3 membranes are promising for the separation of H2O/AcOH mixtures. Given this background, we report, for the first time, the synthesis of c-plane-aligned dense NP-h-WO3 membranes on porous ceramic supports via the hydrothermal method using a precursor solution containing AcOH. The presence of AcOH and the concentration of Na2WO4 in the precursor solution are the key factors affecting crystal growth and alignment along the c-plane. A high Na2WO4 concentration is necessary for obtaining membranes with a high degree of c-plane alignment. Thus, dense, c-plane-aligned NP-h-WO3 membranes could be fabricated by precoating the support with amorphous WO3 seeds and subsequent hydrothermal synthesis in a precursor solution of Na2O/WO3/AcOH/H2O (1/1/0.88/201) at 180 °C for 24 h. The fabricated membranes exhibited a maximum separation factor of 42.6 during the pervaporation of a H2O/AcOH mixture (10/90 (w/w)) at 80 °C. Thus, these NP-h-WO3 membranes are highly suited for H2O/AcOH separation.

DOI： 10.1016/j.memsci.2020.118860

Electrodeposition of nano-diamond/copper composite platings: Improved interfacial adhesion between diamond and copper via formation of silicon carbide on diamond surface 査読有り国際誌

Hagio Takeshi, Park Jae-Hyeok, Naruse Yuto, Goto Yasuki, Kamimoto Yuki, Ichino Ryoichi, Bessho Takeshi

Surface and Coatings Technology 403 巻 2020年12月

Removal of heavy metals by BEA zeolite/Fe<inf>3</inf>O<inf>4</inf> composite prepared via dry-gel conversion method using agrowaste-derived raw material 査読有り国際共著国際誌

Phouthavong V., Hagio T., Park J.H., Nijpanich S., Duangkhai K., Rujiravanit R., Thaveemas P., Chounlamany V., Kong L., Li L., Ichino R.

Solid State Sciences 149 巻 2024年3月

担当区分：責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Solid State Sciences

Using agrochemicals are considered as an anthropogenic source of heavy metal contamination in water, and ecofriendly remediation tools for removal is desired. Here, we demonstrate material circulation by converting SiO2 extracted from agrowaste: rice husk ash, into an easily collectable adsorbent: BEA zeolite/Fe3O4 composite, through dry-gel conversion technique. In addition, the synthesized BEA zeolite/Fe3O4 composite was tested for removal of heavy metals for the first time. Instrumental analyses confirmed that incorporated Fe3O4 particles inside BEA zeolites showed no severe effects on its morphologies. Pseudo-second order kinetic and Langmuir isotherm models were found best described the adsorption of three typical toxic heavy metals: Pb(II), Cu(II), Zn(II). Moderate adsorption capacities of 0.675, 0.310, and 0.308 mmol/g for Pb(II), Cu(II), and Zn(II), respectively, following the selectivity order: Pb(II) > Cu(II) ≈ Zn(II) were obtained. The composite adsorbent exhibits magnetic collectability, reusability and stability, indicating its practicality for removal of heavy metals from water.

DOI： 10.1016/j.solidstatesciences.2024.107473

Super hardening of Fe–W alloy plating by phase transformation of amorphous to metal carbides-dispersed nanocrystalline alloys and application as promising alternative for hard chromium plating 査読有り国際共著国際誌

Park J.H., Kim J.I., Shinohara Y., Hagio T., Umehara N., Ichino R.

Surface and Coatings Technology 477 巻 2024年2月

担当区分：責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Surface and Coatings Technology

Despite the superior hardness, wear resistance, and corrosion resistance of hard chromium (Cr) plating using toxic hexavalent chromium (Cr6+), the gradual restriction on the use of Cr6+ in industrial fields necessitates the development of an alternative, harmless plating material with excellent performance. Here, we report the fabrication of super-hard plating by the simple annealing of electrodeposited Fe–W–C plating as a promising alternative for hard Cr plating. Amorphous-structured Fe–W–C plating, including co-deposited citric acid-derived carbon, forms uniformly dispersed ternary metal carbides inside the plating during annealing, which changes the plating structure from amorphous to nano-carbide-dispersed alloys. The phase-transformed, nanocrystalline Fe–W–C alloy annealed at 700 °C exhibited a maximum hardness of 20.5 GPa, which surpassed the hardness of hard Cr plating (12.5 GPa). The ball-on-disc tribo-test and corrosion test results further demonstrated the superior wear and anti-corrosion properties of the carbide-dispersed Fe–W–C alloy plating compared with hard Cr plating. This study develops the applicability of this super-hard plating as a new hard coating material that overcomes the limitations of conventional metal plating without using any toxic chemical.

DOI： 10.1016/j.surfcoat.2024.130388

Nanoarchitectonics Solution Plasma Polymerization of Amino-Rich Carbon Nanosorbents for Use in Enhanced Fluoride Removal 査読有り国際誌

Tipplook, M; Tanaka, H; Sudare, T; Hagio, T; Saito, N; Teshima, K

ACS APPLIED MATERIALS & INTERFACES 16 巻 ( 6 ) 頁： 7038 - 7046 2024年2月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：ACS Applied Materials and Interfaces

Amino-functionalized carbon (NH2C) is an effective adsorbent in removing pollutants from contaminated water because of its high specific surface area and electrical charge. In the conventional preparation method, the introduction of amino groups onto the carbon surface is limited, resulting in low pollutant adsorption. Herein, we present simultaneous carbonization and amination to form NH2C via electrical discharge of nonequilibrium plasma, and the resultant material is applied as an effective adsorbent in fluoride removal. The simultaneous process introduces numerous amino groups into the carbon framework, enhancing the adsorption efficiency. The fluoride adsorption capacity is approximately 121.12 mg g-1, which is several times higher than those reported in previous studies. Furthermore, computational modeling is performed to yield deeper mechanistic insights into the molecular-level adsorption behavior. These data are useful in designing and synthesizing advanced materials for applications in water remediation.

DOI： 10.1021/acsami.3c15172

c面配向六方晶酸化タングステン膜の分子ふるい型分離膜としての可能性招待有り査読有り国際共著

萩尾健史, 國司寛人, 和田慎太郎, 寺尾年弘, 木下空, プッタヴーンワンパサート, ニッチパーニッチスーピンヤー, パクジェヒョク, 市野良一

ゼオライト 41 巻 ( 1 ) 頁： 9 - 19 2024年1月

担当区分：筆頭著者,　責任著者記述言語：日本語掲載種別：研究論文（学術雑誌）出版者・発行元：一般社団法人日本ゼオライト学会

カーボンニュートラルおよび持続可能な社会の実現に向け，エネルギー消費の大きい分離プロセスの省エネルギー化や資源循環に貢献する分離膜は益々注目されている。その中で，膜材料の検討は分離特性を決定づける重要な研究要素の一つである。分子サイズのミクロ細孔を有する無機結晶（ミクロ多孔無機結晶）は分子ふるいとも呼ばれる有望な分離膜材料である。筆者らは，この分子ふるい型膜材料として新たに六方晶酸化タングステンの可能性を提案してきた。同材料は，結晶のc軸と並行な一軸細孔を有するため，そのc面配向膜は分子ふるい型分離膜として機能すると予想されるが，分離膜材料としては検討されてこなかった。本稿では，筆者らが種々の対策によって緻密なc面配向六方晶酸化タングステン膜の合成に挑戦し，液分離並びにガス分離への適用可否を検討した結果を紹介する。得られた膜は，水／酢酸の混合溶液から水を選択的に分離できることが確認された。また，各種液およびガス分子の透過特性を調査した結果，ミクロ細孔を利用した小分子向けの分子ふるい型分離膜として機能するであろうことを見出した。本発見は膜材料の選択肢拡大に寄与すると期待される。

DOI： 10.20731/zeoraito.41.1.9

Effects of the Topological Structure of Different Cu-Zeolites on the Relationship between Soot and NO<sub>x</sub> Removal on NH<sub>3</sub>-SCRF 査読有り国際共著国際誌

Ye, ZM; Zhao, PC; Tang, XC; Hagio, T; Sato, K; Nagaoka, K; Li, XL

ENERGY & FUELS 38 巻 ( 3 ) 頁： 2212 - 2223 2024年1月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Energy and Fuels

Experimental studies were carried out to explore the effect of zeolite topology on NOx purification and soot oxidation in ammonia selective catalytic reduction coated diesel particulate filter (SCRF) catalysts. The catalytic activity of Cu-exchanged zeolites Cu/SSZ-13 (CHA topology), Cu/ZSM-5 (MFI), and Cu/BEA(BEA) was evaluated in the NH3-SCRF. Experiments with XRD and ICP-SFMS demonstrated that the three types of samples retained their typical structural peaks after Cu modification, and the similar ratios of Cu/Al and Si/Al ensure that the primary cause of different catalytic performances was caused by different framework structures. As determined by laboratory experiments with synthetic gas, Cu/SSZ-13 exhibited an extended activity window and a higher deNOx efficiency at NO2/NOx below 0.5. In addition, Cu/ZSM-5 consistently exhibited superior CO2 selectivity in soot-loading experiments, regardless of the NO2 concentration. When loaded with soot, Cu/BEA exhibited exceptional deNOx performance at NO2/NOx = 0.5. NH3 was observed to have a negative effect on soot oxidation by NO2, while the consumption of NO2 by soot oxidation contributed to the NO2-SCR reaction being aided. Influenced by different zeolite structural features, the degree of diffusion of copper in the zeolite as well as the replacement sites are different, thus forming different ratios of copper species. For instance, the presence of Z2Cu sites, which can adsorb more NH3 molecules than ZCuOH sites as indicated by the in situ DRIFTS results, and the presence of Cu+ with stronger redox properties compared to Cu2+, can be influenced by these structural characteristics. Additionally, soot particles have the ability to act as adsorption sites for the NH3-SCR reaction.

DOI： 10.1021/acs.energyfuels.3c03034

AC Electromagnetic Field Controls the Biofilms on the Glass Surface by Escherichia coli & Staphylococcus epidermidis Inhibition Effect 査読有り国際共著国際誌

Aoyama, N; Kanematsu, H; Barry, DM; Miura, H; Ogawa, A; Kogo, T; Kawai, R; Hagio, T; Hirai, N; Kato, T; Yoshitake, M; Ichino, R

MATERIALS 16 巻 ( 21 ) 2023年11月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Materials

Biofilms, mainly comprised of bacteria, form on materials’ surfaces due to bacterial activity. They are generally composed of water, extracellular polymeric substances (polysaccharides, proteins, nucleic acids, and lipids), and bacteria. Some bacteria that form biofilms cause periodontal disease, corrosion of the metal materials that make up drains, and slippage. Inside of a biofilm is an environment conducive to the growth and propagation of bacteria. Problems with biofilms include the inability of disinfectants and antibiotics to act on them. Therefore, we have investigated the potential application of alternating electromagnetic fields for biofilm control. We obtained exciting results using various materials’ specimens and frequency conditions. Through these studies, we gradually understood that the combination of the type of bacteria, the kind of material, and the application of an electromagnetic field with various low frequencies (4 kHz–12 kHz) changes the circumstances of the onset of the biofilm suppression effect. In this study, relatively high frequencies (20 and 30 kHz) were applied to biofilms caused by Escherichia coli (E. coli) and Staphylococcus epidermidis (S. epidermidis), and quantitative evaluation was performed using staining methods. The sample surfaces were analyzed by Raman spectroscopy using a Laser Raman spectrometer to confirm the presence of biofilms on the surface.

DOI： 10.3390/ma16217051

Synthesis of Sulfur-Doped Magnetic Iron Oxides for Efficient Removal of Lead from Aqueous Solutions 査読有り国際共著国際誌

Xu, JQ; Pan, MT; Zou, C; Huang, XQ; Hagio, T; Ichino, R; Kong, L; Li, L

WATER 15 巻 ( 20 ) 2023年10月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Water (Switzerland)

Heavy metal pollution poses an environmental risk, and its efficient removal and facile separation from water remains a challenge. Magnetic iron oxide, an eco-friendly, relatively stable, and easy-separation material, has been regarded as one of the most applicable adsorbents for water treatment. However, the limited adsorption capacity has restricted its applications. Herein, sulfur-doped magnetic Fe3O4 (Sx–Fe3O4) adsorbent was fabricated using a calcination method for the efficient removal of Pb(II) from water. In contrast to undoped Fe3O4, the introduction of doped sulfur greatly enhanced the adsorption performance of S–Fe3O4 over four times, with a maximum capacity of 333.33 mg g−1, which was synthesized at 300 °C with a raw molar ratio of S–Fe of 5. Based on the structure and morphology analysis, it was demonstrated that sulfur was successfully doped into the Fe3O4 structures, which resulted in Fe3O4 with active sulfur sites accordingly contributing to the adsorption enhancement through the combination of strong soft–soft interactions between soft base sulfur and soft acid Pb(II) along with surface adsorption. Sx–Fe3O4 could maintain the adsorption performance in the presence of competing ions. Furthermore, although the sulfur doping process exhibited slight side effects on the magnetic property, magnetic Sx–Fe3O4 maintained the high separation potential. This study presented a promising strategy to enhance the adsorption performance of Fe3O4 through sulfur doping for Pb(II) removal from water.

DOI： 10.3390/w15203667

Preparation and Characterization of TiO(2)-Coated Hollow Glass Beads for Functionalization of Deproteinized Natural Rubber Latex via UVA-Activated Photocatalytic Degradation. 査読有り国際共著国際誌

Nijpanich S, Nimpaiboon A, Rojruthai P, Park JH, Hagio T, Ichino R, Sakdapipanich J

Polymers 15 巻 ( 19 ) 2023年9月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Polymers

The photochemical degradation of natural rubber (NR) is a prevalent method used to modify its inherent properties. Natural rubber, predominantly derived from the Hevea Brasiliensis tree, exhibits an exceptionally high molecular weight (MW), often reaching a million daltons (Da). This high MW restricts its solubility in various solvents and its reactivity with polar compounds, thereby constraining its versatile applications. In our previous work, we employed TiO2 in its powdered form as a photocatalyst for the functionalization of NR latex. However, the post-process separation and reuse of this powder present substantial challenges. In this present study, we aimed to functionalize deproteinized NR (DPNR) latex. We systematically reduced its MW via photochemical degradation under UVA irradiation facilitated by H2O2. To enhance the efficiency of the degradation process, we introduced TiO2-coated hollow glass beads (TiO2-HGBs) as photocatalysts. This approach offers the advantage of easy collection and repeated reuse. The modified DPNR showed a reduction in its number-average MW from 9.48 × 105 to 0.28 × 105 Da and incorporated functional groups, including hydroxyl, carbonyl, and epoxide. Remarkably, the TiO2-HGBs maintained their performance over seven cycles of reuse. Due to their superior efficacy, TiO2-HGBs stand out as promising photocatalysts for the advanced functionalization of NR across various practical applications.

DOI： 10.3390/polym15193885

Room-Temperature Bulk Supramolecular Polymer Based on C<inf>3</inf>-Symmetrical Benzene-1,3,5-tricarboxamides Having Two-Armed Alkyl Groups as Side Chains 査読有り国際誌

Ishigaki Y., Yamanaka M., Hagio T., Ichino R.

ChemistrySelect 8 巻 ( 35 ) 2023年9月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：ChemistrySelect

To develop a bulk supramolecular polymer based on 1,3,5-benzenetricarboxamide (BTA) without crystallinity at room temperature, C3-synmetrical BTA derivatives with two-armed alkyl groups were synthesized and characterized. IR and XRD measurements of the BTA derivatives suggested that the higher-order structure obtained using these materials was hexagonal columnar, owing to the characteristic three-fold hydrogen bonding. In DSC measurements, BTA having 10-nonadecyl groups (10NDBTA) showed only a single transition point at 233 °C and maintained its mesophase down to −50 °C, whereas the other BTA derivatives showed a transition peak in the range of 20 to 131 °C and another in the range of 204 to 239 °C, corresponding to alkyl melting and dissociation of the stacked BTA cores, respectively. 13C-SSNMR measurement of 10NDBTA indicated that not only the 10-nonadecyl groups of the side chains but also the BTA cores forming the main chain of the supramolecular polymer show a unique high mobility even at ambient temperature.

DOI： 10.1002/slct.202300805

Gas permeation properties of c-plane aligned hexagonal tungsten oxide membranes formed by multi-stage synthesis 査読有り国際共著国際誌

Wada Shintaro, Hagio Takeshi, Kunishi Hiroto, Park Jae-Hyeok, Phouthavong Vanpaseuth, Yamada Yuta, Terao Toshihiro, Li Xinling, Nijpanich Supinya, Ichino Ryoichi

JOURNAL OF THE KOREAN CERAMIC SOCIETY 2023年8月

担当区分：責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Journal of the Korean Ceramic Society

Crystalline microporous membranes are promising tools for gas separation because their molecular dimension pores allow us to accurately sieve molecules by size. Recently, microporous hexagonal WO3 was reported as a new potential membrane material and its membrane was found to enable separation of water from water/acetic acid mixtures. Pore size of hexagonal WO3 seemed to be also suitable for separation of small gasses; however, its gas permeation properties have not been reported. Additionally, densification of membranes by decreasing intercrystalline gaps are extremely important in gas separation. One effective method to densify polycrystalline membranes is to repeat membrane synthesis, namely multi-stage synthesis. Here, we attempt to prepare dense hexagonal WO3 membranes on porous tubular supports by multi-stage synthesis and examined their densification and gas permeation properties. Densification was confirmed by permeation of SF6 (gas molecule larger than pores of hexagonal WO3), and its potential for separating small gasses was considered from single gas permeation of He and He/SF6 permselectivity. The results indicated that the multi-stage synthesis is effective to densify the membranes and He/SF6 permselectivity reached 42.8 for three-stage synthesis under modified conditions, implying hexagonal WO3 is a potential membrane material for small gas separation.

DOI： 10.1007/s43207-023-00321-5

An effective strategy for improving the performance of electrodeposited Fe-W alloy plating: Tailoring microstructure by graphene incorporation 査読有り国際共著国際誌

Shinohara Yu, Park Jae-Hyeok, Hagio Takeshi, Kim Jae-Il, Lee Woo-Young, Umehara Noritsugu, Ichino Ryoichi

MATERIALS & DESIGN 230 巻 2023年6月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Materials and Design

Despite the excellent performance of hard Cr plating using hexavalent chromium (Cr6+), its use is being restricted owing to recent environmental regulations. Electrodeposited Fe-W alloy is considered a possible alternative, but its high coefficient of friction (COF), high wear rate owing to tribo-oxidation, and high corrosion rate hinder its practical application. In this study, we attempted to solve these problems by modifying the microstructure of Fe-W alloy by incorporating 2D-structured graphene. The effect of graphene incorporation on the structure of the Fe-W alloy and its properties, especially microhardness, wear, and corrosion resistance, were investigated. The results showed the graphene effectively modified the columnar structure of the Fe-W alloy by inhibiting the vertical growth of clusters during electrodeposition, leading to fragmentation of the vertical cluster boundaries. This improved the hardness by as much as 17 % up to 9.1 GPa, and the corrosion resistance by changing the corrosion mechanism from localized corrosion to uniform corrosion. In addition, the graphene reduced the COF and wear rate by reducing the Fe2O3 formed by tribo-oxidation to a lower oxidation state. The structural modification of the plating by graphene incorporation thus provides an effective solution to improving the performance of Fe-W alloys.

DOI： 10.1016/j.matdes.2023.111938

Improvement in the corrosion resistance of electrodeposited Ni-W alloy by MWCNT co-deposition and prevention of metal-carbon interfacial corrosion by carbide formation 査読有り国際誌

Park Jae-Hyeok, Hagio Takeshi, Ichino Ryoichi

JOURNAL OF ALLOYS AND COMPOUNDS 939 巻 2023年4月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Journal of Alloys and Compounds

Composite plating is an effective method which can enhance the properties of conventional metal plating by co-deposition of composite materials. In this study, multi-walled carbon nanotubes (MWCNTs) were used as a composite material to improve the corrosion resistance of Ni-W alloys, and the effect of the MWCNTs addition on the anti-corrosion properties was discussed. The corrosion current density of the Ni-W/MWCNTs composite decreased approximately 4 times from 16.6 to 4.6 μA·cm-2 in 3 wt% NaCl solution compared to the pristine Ni-W; this showed that the co-deposition of MWCNTs was effective for improvement in the corrosion resistance. However, the interfacial corrosion between the metal matrix and MWCNTs occurred in the high potential region and degraded the passivation properties of plating. This interfacial corrosion is caused by the high O content due to the hydroxyl groups on the acid-treated MWCNTs surface and the difference in W concentration between the interface of MWCNTs and the Ni-W matrix. Heat treatment in Ar atmosphere removes these hydroxyl groups and diffuses Ni and W into MWCNTs to form metal carbide (Ni6W6C), effectively alleviating interfacial corrosion. This study presents interfacial corrosion can be effectively mitigated by forming metal carbides at the interface of carbon materials in metal/carbon composites.

DOI： 10.1016/j.jallcom.2023.168788

Preliminary Study on Electrodeposition of Copper Platings and Codeposition of Carbon Nanotubes from Organic Solvent 査読有り国際共著国際誌

Park Jae-Hyeok, Fujita Yusei, Hagio Takeshi, Phouthavong Vanpaseuth, Kamimoto Yuki, Bessho Takeshi, Ichino Ryoichi

COATINGS 13 巻 ( 4 ) 2023年4月

担当区分：責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Coatings

Metal/carbon composite plating is an effective strategy for improving and adding properties to metal plating by incorporating carbon materials into the metal matrices. Copper (Cu) is widely applied, particularly in the areas of heat management and electronic packaging owing to its high thermal and electrical conductivities, which can be further improved together with improvements in mechanical properties by compositing it with carbon nanotubes (CNTs). However, because hydrophobic CNTs are hardly dispersible in aqueous solutions, additional intense acid treatment or the addition of dispersants is required for their dispersion. Moreover, previous studies have reported that these methods suffer from deterioration of composite material performance through the destruction of the CNT surface or the inclusion of dispersants into the plating. Therefore, in this study, the electrodeposition of a Cu/CNT composite in a non-aqueous solvent that can disperse CNTs without any additional treatment is investigated. The experimental results show that it is possible to deposit Cu from a N-methyl-2-pyrrolidone containing copper iodide and potassium iodide. Furthermore, Cu/CNT composite platings containing CNTs up to 0.12 mass% were prepared by constant current electrolysis, and applying pulse electrolysis can increase the CNTs content up to 0.22 mass%.

DOI： 10.3390/coatings13040802

Effect of nanostructure, porosity and extent of oxidation on soot reactivity 査読有り国際共著国際誌

Fang Mingming, Zhao Pengcheng, Ma Yongzhi, Hagio Takeshi, Li Xinling

FULLERENES NANOTUBES AND CARBON NANOSTRUCTURES 31 巻 ( 3 ) 頁： 241 - 254 2023年3月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Fullerenes Nanotubes and Carbon Nanostructures

Oxidation evolutions of structure, porosity and reactivity properties of four model carbons (PU, S160, N330 and R250) with different initial reactivity were studied. Results showed that changes in the porosity and nanostructure properties instead of initial properties significantly affected the soot reactivity during the soot oxidation process. Two high-reactivity soot surrogate samples, i.e., PU and S160, initially presented turbostratic disordered crystallites, resulting in higher reactivity at the early oxidation stage. Oxidation mainly proceeded inwardly in a peeling fashion, and more disordered internal crystallites were exposed after oxidized, slightly increasing the reactivity of PU and S160. Two low reactivity soot surrogate samples, i.e., N330 and R250, initially exhibited the typical core–shell structure. The oxidation rates of N330 and R250 were lower than that of PU and S160 due to more ordered exterior crystallites and less surface oxygen content at the early oxidation stage. Once oxygen penetrated the particle core, many pores were generated. Next, the particle became hollow through internal burning of the more reactive internal carbon at the late oxidation stage. After 40% burnoff, these hollow structures promoted oxidation in both outward and inward directions. Therefore, oxidation rates of N330 and R250 significantly increased.

DOI： 10.1080/1536383X.2022.2139371

Facile Synthesis of Spherical Porous Tricobalt Tetroxide and Metal Cobalt for High Quality Cobalt Production and Recycling 査読有り国際誌

Matsunaga, S; Suzuki, T; Hagio, T; Park, JH; Kamimoto, Y; Ichino, R; Takeshita, K; Sato, F; Sasaya, K; Iguchi, T; Tsunekawa, M

MATERIALS TRANSACTIONS 64 巻 ( 12 ) 頁： 2739 - 2747 2023年

担当区分：責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Materials Transactions

Liquid-phase synthesis is suitable for controlling the morphological and structural properties of functional inorganic materials and such control is important because they strongly affect the functionality of the product. Cobalt-based materials is one group of materials that requires control of powder morphology and structure. Cobalt is an important metal element used in various industrial fields such as secondary batteries, superalloys, permanent magnets, hard metals, and catalysts. The ever-growing demand of cobalt highlights that there is an urgent necessity to develop high quality material synthesis methods and to secure cobalt resources for countries that rely on import like Japan. Especially, technologies to recycle cobalt in a form reusable for secondary batteries and catalysts are desired because further increase in demand is anticipated. Meanwhile, spherical porous tricobalt tetroxide secondary particles obtained by calcination of spherical cobalt carbonate precursors have been reported to be promising materials for battery applications. Moreover, porous metal cobalt obtained by hydrogen reduction of tricobalt tetroxide is known to be effective for catalyst applications. However, conventional methods to synthesize spherical cobalt carbonate requires addition of additives in the reaction mixtures or otherwise requires hydrothermal treatment in pressure vessels. These are unfavorable to develop a practical and sustainable process for cobalt-based material production and recycling. In this study, a facile room temperature synthesis method to prepare spherical cobalt carbonate precursors from solutions of cobalt chloride and ammonium hydrogen carbonate that does not require any additives or hydrothermal treatment is developed by optimizing the carbonate solution concentration, carbonate/cobalt salt molar ratio, and stirring time during reaction. Furthermore, we succeeded in obtaining porous tricobalt tetroxide and porous metal cobalt that carry on the exterior spherical morphology of the original cobalt carbonate precursor by calcination and hydrogen reduction. The developed process shall contribute to realize high quality cobalt-based material production and recycling.

DOI： 10.2320/matertrans.M-M2023809

Oxidation evolutions of soot surface and pore properties with different O-2-NO2 mixtures and temperatures 査読有り国際共著国際誌

Ma Yongzhi, Zhao Pengcheng, Fang Mingming, Hagio Takeshi, Li Xinling

FULLERENES NANOTUBES AND CARBON NANOSTRUCTURES 30 巻 ( 10 ) 頁： 1066 - 1074 2022年10月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Fullerenes Nanotubes and Carbon Nanostructures

Soot oxidation evolutions at various oxidation degrees under different O2-NO2 mixtures and temperatures were performed. Results indicated that the internal burning-out process represented by shell-like particles at 500 °C independent on NO2 concentration, while the development of hollow shells for the soot was suppressed with increasing the temperature. A tendency with soot toward a less ordered arrangement with short and defective graphene layers after oxidizing at 500 °C was also observed, which was suppressed with added NO2 and increasing temperature. Many carbon oxygen functionalities produced at 40% oxidation and the intensity of the peak gradually increased as the increase of the oxidation degree, while the increase of the peak intensity became less sensitive with added NO2 and increasing temperature. Abundant micropores and mesopores formed inside the particles during the soot oxidation process depending on oxidizer and temperature, micropores (smaller than 2 nm) were extensively generated at the early stages of the oxidation while mesopores increased sharply after 20% oxidation. The trends were correspondent to the oxidation modes with different oxidizer and temperature. The correlationship observation suggested that soot oxidation behavior was dependent on competing rates of reaction kinetics versus mass transport of oxidizer according to the oxidation evolution of surface and pore.

DOI： 10.1080/1536383X.2022.2072831

Aluminum Electrodeposition on the Surface of Boron Carbide Ceramics by Use EMIC-AlCl3 Ions Liquid 査読有り国際誌

Gou Roujia, Park Jae-Hyeok, Yamashita Seiji, Hagio Takeshi, Ichino Ryoichi, Kita Hideki

COATINGS 12 巻 ( 10 ) 2022年10月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Coatings

Coating technology is decisively important for metallization of ceramic materials and ceramic metal sealing technology. Previous studies have shown that the network-like structure after penetration of molten aluminum can significantly improve the strength of joint components. However, the direct aluminum coating method is limited by the shape of the substrate. To obtain a dense aluminum film on the surface of B4C, in this study, aluminum was deposited by pulse electroplating in EMIC–AlCl3 ionic liquid. The deposited metals were observed and analyzed by SEM–EDS and XRD. A Vickers hardness tester was adopted as an auxiliary equipment to clarify the film quality. The results show that frequency and duty cycle have significant effects on crystal orientation. The content of oxides in the contact gap reduces the bonding strength of the deposited metal, which provides experimental basis for metal electrodeposition on B4C.

DOI： 10.3390/coatings12101535

Facile synthesis of amine-functionalized three-dimensional graphene composites for CO2 capture 査読有り国際共著国際誌

Sun Hefei, Zhang Qinggang, Hagio Takeshi, Ryoichi Ichino, Kong Long, Li Liang

SURFACES AND INTERFACES 33 巻 2022年10月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Surfaces and Interfaces

Excessive emissions of carbon dioxide (CO2) cause the greenhouse effect. CO2 capture and storage has been recognized as an important solution for reducing carbon dioxide emissions and coping with global warming. The synthesis of porous materials for effective CO2 adsorption is considered to be one of the most possible methods for CO2 capture and storage at present, however, achieving selective and efficient CO2 adsorption and conversion is still quite a challenge. Herein, a series of three-dimensional graphene-based materials (3D GBMs) were synthesized by alkali metal involved method, which showed high specific surface area (477.56 m2 g−1–792.96 m2 g−1) and abundant micropore and mesopore surface structures. We demonstrated that introducing N-containing or O-containing functional groups into the carbon framework can create more surface microporous structures and active adsorption sites, and significantly enhance the CO2 adsorption performance of 3D GBMs. Furthermore, it was found that the simultaneously introduction of the two kinds of functional groups into 3D GBMs could further increase the adsorption capacity of CO2 (from 2.06 mmol g−1 to 4.79 mmol g−1). All the above results indicate the treated 3D GBMs could have a great potential as efficient adsorbent in CO2 capture and storage.

DOI： 10.1016/j.surfin.2022.102256

Amine-Modified Small Pore Mesoporous Silica as Potential Adsorbent for Zn Removal from Plating Wastewater 査読有り国際誌

Phouthavong Vanpaseuth, Park Jae-Hyeok, Nishihama Tatsuo, Yoshida Shuhei, Hagio Takeshi, Kamimoto Yuki, Ichino Ryoichi

COATINGS 12 巻 ( 9 ) 2022年9月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Coatings

The removal of Zn from wastewater generated from the Zn-based electroplating manufacturing process is essential because the regulation limit of Zn concentration in wastewater is becoming stricter in Japan. However, achieving this through conventional methods is difficult, especially for small and medium enterprises in the plating industry. Therefore, a suitable Zn-removal method with a low cost but high performance and Zn selectivity is required. The application of adsorbents is one possible solution. Mesoporous silica (MS) is a well-known adsorbent with controllable pore size, high specific surface area (SSA), high acid resistance, and ease of surface modification. In this study, we modified the surfaces of MSs with different initial pore sizes by amino groups and investigated their Zn removal performances. The effect of pore size on amine modification using (3-aminopropyl)triethoxysilane and on adsorption performance in a single system was investigated along with Zn adsorption selectivity in the Zn–Ni binary system. Amine-modified MS prepared from MS with an initial pore size of 1.9 nm showed drastically lower performance compared to those prepared from MS with an initial pore size larger than 2.8 nm. Zn-selectivity in the Zn–Ni binary system, containing equal amounts of Zn and Ni, was found to reach a maximum of 21.6 when modifying MS with an initial pore size of 2.8 nm.

DOI： 10.3390/coatings12091258

Effect of Zn-Mg interlayer on the corrosion resistance of multilayer Zn-based coating fabricated by physical vapor deposition process 査読有り国際共著国際誌

Park J.H., Ko K.P., Hagio T., Ichino R., Lee M.H.

Corrosion Science 202 巻 2022年7月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Corrosion Science

A novel Zn/Zn-Mg/Zn multilayer coating is prepared on steel plate by PVD. The effect of the multilayer structure comprising Zn-Mg interlayer on the corrosion resistance is discussed. The corrosion resistance is evaluated by the salt spray test, and the corrosion progression is analyzed by electrochemical impedance spectroscopy and corrosion products observation. Eluted Mg ions from the Zn-Mg interlayer form a porous Mg corrosion product layer that permeates chlorine ions, assists the coating transform to Zn5(OH)8Cl2·H2O phase. Improved corrosion resistance of the coating can be explained by the rapid increasement of the impedance by the formation of the protective Zn5(OH)8Cl2·H2O phase.

DOI： 10.1016/j.corsci.2022.110330

Impedance Characteristics of Monolayer and Bilayer Graphene Films with Biofilm Formation and Growth. 査読有り国際共著国際誌

Nakagawa R, Saito K, Kanematsu H, Miura H, Ishihara M, Barry DM, Kogo T, Ogawa A, Hirai N, Hagio T, Ichino R, Ban M, Yoshitake M, Zimmermann S

Sensors (Basel, Switzerland) 22 巻 ( 9 ) 2022年5月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Sensors

Biofilms are the result of bacterial activity. When the number of bacteria (attached to materials’ surfaces) reaches a certain threshold value, then the bacteria simultaneously excrete organic polymers (EPS: extracellular polymeric substances). These sticky polymers encase and protect the bacteria. They are called biofilms and contain about 80% water. Other components of biofilm include polymeric carbon compounds such as polysaccharides and bacteria. It is well-known that biofilms cause various medical and hygiene problems. Therefore, it is important to have a sensor that can detect biofilms to solve such problems. Graphene is a single-atom-thick sheet in which carbon atoms are connected in a hexagonal shape like a honeycomb. Carbon compounds generally bond easily to graphene. Therefore, it is highly possible that graphene could serve as a sensor to monitor biofilm formation and growth. In our previous study, monolayer graphene was prepared on a glass substrate by the chemical vapor deposition (CVD) method. Its biofilm forming ability was compared with that of graphite. As a result, the CVD graphene film had the higher sensitivity for biofilm formation. However, the monolayer graphene has a mechanical disadvantage when used as a biofilm sensor. Therefore, for this new research project, we prepared bilayer graphene with high mechanical strength by using the CVD process on copper substrates. For these specimens, we measured the capacitance component of the specimens’ impedance. In addition, we have included a discussion about the possibility of applying them as future sensors for monitoring biofilm formation and growth.

DOI： 10.3390/s22093548

Simultaneous reduction and sequestration of hexavalent chromium by magnetic β-Cyclodextrin stabilized Fe<sub>3</sub>S<sub>4</sub>. 査読有り国際共著国際誌

Kong L, Yan R, Liu M, Xu J, Hagio T, Ichino R, Li L, Cao X

431 巻頁： 128592 2022年2月

Magnetic Adsorbents for Wastewater Treatment: Advancements in Their Synthesis Methods 査読有り国際共著国際誌

Phouthavong V., Yan R., Nijpanich S., Hagio T., Ichino R., Kong L., Li L.

Materials 15 巻 ( 3 ) 2022年2月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：MDPI

The remediation of water streams, polluted by various substances, is important for realizing a sustainable future. Magnetic adsorbents are promising materials for wastewater treatment. Although numerous techniques have been developed for the preparation of magnetic adsorbents, with effective adsorption performance, reviews that focus on the synthesis methods of magnetic adsorbents for wastewater treatment and their material structures have not been reported. In this review, advancements in the synthesis methods of magnetic adsorbents for the removal of substances from water streams has been comprehensively summarized and discussed. Generally, the synthesis methods are categorized into five groups, as follows: direct use of magnetic particles as adsorbents, attachment of pre-prepared adsorbents and pre-prepared magnetic particles, synthesis of magnetic particles on pre-prepared adsorbents, synthesis of adsorbents on preprepared magnetic particles, and co-synthesis of adsorbents and magnetic particles. The main improvements in the advanced methods involved making the conventional synthesis a less energy intensive, more efficient, and simpler process, while maintaining or increasing the adsorption performance. The key challenges, such as the enhancement of the adsorption performance of materials and the design of sophisticated material structures, are discussed as well.

DOI： 10.3390/ma15031053

光触媒を用いたダイヤモンドのアミノ基修飾と銅基質に対する高分散複合化技術査読有り

加藤華月, 石田直哉, 鈴木孝宗, 藤本憲次郎, 萩尾健史, 市野良一, 近藤剛史, 湯浅真, 上塚洋, 藤嶋昭, 寺島千晶

表面技術 72 巻 ( 12 ) 頁： 701 - 703 2021年12月

記述言語：日本語掲載種別：研究論文（学術雑誌）出版者・発行元：一般社団法人表面技術協会

<p>We strove to produce a microdiamond（MD）- copper composite by electroplating. Unfortunately, copper is naturally non-wetting with MD because of their chemical incompatibility. We achieved modification of the amino group for the MD surface using a photocatalytic treatment, followed by electroplating of the copper. Results demonstrated that the MD - copper composite material assisted by photocatalysis markedly improved their interfacial affinity and thermal conductivity.</p>

DOI： 10.4139/sfj.72.701

Synthesis of 3D graphene-based materials and their applications for removing dyes and heavy metals 査読有り国際共著国際誌

Sun Hefei, Lin Yan, Takeshi Hagio, Wang Xinze, Wu Deyi, Tian Yanqin

ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH 28 巻 ( 38 ) 頁： 52625 - 52650 2021年10月

Preparation of amino group functionalized diamond using photocatalyst and thermal conductivity of diamond/copper composite by electroplating 査読有り国際誌

Ishida Naoya, Kato Kazuki, Suzuki Norihiro, Fujimoto Kenjiro, Hagio Takeshi, Ichino Ryoichi, Kondo Takeshi, Yuasa Makoto, Uetsuka Hiroshi, Fujishima Akira, Terashima Chiaki

DIAMOND AND RELATED MATERIALS 118 巻頁： 108509 2021年10月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Diamond and Related Materials

We focused on a micro diamond (MD) particle with the highest thermal conductivity among existing materials and aimed to make a MD/copper composite material by electroplating. However, copper is naturally non-wetting with MD due to its chemical incompatibility, leading to weak interfacial bonding and high thermal resistance. We improved the wettability between MD and copper functionalized by the amino group on the MD using a photocatalytic reaction. The functionalization of the diamond surface by amino groups was achieved by treating the MDs in a 3-aminopropyltrimethoxysilane-containing solution. The amino group functionalized MD was dispersed in the electroplating bath, where copper was deposited on the MD. As a result, the composite material of amino group functionalized MD assisted by photocatalyst and copper improved their interfacial affinity and exhibited the high thermal conductivity of 595 W/m K.

DOI： 10.1016/j.diamond.2021.108509

Evenly distribution of amorphous iron sulfides on reconstructed Mg-Al hydrotalcites for improving Cr(VI) removal efficiency 査読有り国際共著国際誌

Yan Ruixin, Feng Xiuping, Kong Long, Wan Qun, Zheng Weilin, Hagio Takeshi, Ichino Ryoichi, Cao Xinde, Li Liang

CHEMICAL ENGINEERING JOURNAL 417 巻頁： 129228 2021年8月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Chemical Engineering Journal

Hexavalent Chromium (Cr(VI)) in water is a public health concern and has been a challenging research subject in environmental field for many years. Herein, a novel composite material consisting of amorphous iron sulfides supported on hydrotalcites (FeS/HTs) was synthesized by “calcination-reconstruction-calcination” process, which enables homogeneous distribution of iron and sulfur on the surface of hydrotalcites (HT). The composite (mass ratio of FeS/HT was 1/2) could effectively remove over 98% of Cr(VI) within 10 min. A pseudo-second-order kinetic model and a Langmuir isotherm model were well fitted the sorption data with a maximum removal capacity of 206.2 mg/g. The superior adsorption capacity of FeS/HTs could be attributed to the combination of the advantages of abundant adsorption sites on HT and powerful reduction properties of iron sulfides. X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analysis suggested the adsorbed Cr(VI) on the surface and interlayer of FeS/HTs had been reduced to Cr(III) by reductant iron and sulfur. This study demonstrated that FeS/HTs has potential application prospects in Cr(VI) removal.

DOI： 10.1016/j.cej.2021.129228

Electroplating of copper/microdiamond composites and the effect of diamond surface functionalization 査読有り国際誌

Naruse Yuto, Park Jae-Hyeok, Hagio Tkeshi, Kamimoto Yuki, Ichino Ryoichi, Bessho Takeshi

FUNCTIONAL MATERIALS LETTERS 14 巻 ( 05 ) 2021年7月

担当区分：責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Functional Materials Letters

Compositing diamonds with high thermally conductive metals, such as copper, have attracted much attention in recent years. In this study, we prepared copper/diamond composites by electroplating and investigated the effect of the surface functionalization of diamond on the interfacial adhesion of copper and diamond in the composite. Oxygen-containing groups were introduced on the diamond surface by a hydrothermal treatment and amino groups were further introduced using a silane coupling agent. Surface functionalization of diamond with both these groups led to drastically increased wettability against the copper sulfate solution and improved the interfacial adhesion of copper and diamond in the composite. Compared with that of the plating based on pristine diamond, the thermal conductivity of the platings based on diamond functionalized with oxygen-containing groups and amino groups increased by 42 and 31 W m-1 K-1, respectively. Thus, diamond surface functionalization effectively improved the adhesion at the copper/diamond interface in electroplated copper/diamond composites.

DOI： 10.1142/S1793604721510231

Effect of SiC formation temperature on improvement in thermal conductivity of electrodeposited SiC-coated diamond/Cu composite plating 査読有り国際誌

Naruse Yuto, Park Jae-Hyeok, Hagio Takeshi, Kamimoto Yuki, Bessho Takeshi, Ryoichi Ichino

COMPOSITE INTERFACES 2021年6月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Composite Interfaces

Diamond/Cu composites are considered promising heat spreader materials; however, improving the interfacial adhesion between diamond and Cu is a challenge in manufacturing these composites. We focused on the surface modification of diamonds and previously reported that the formation of a SiC on the diamond surface effectively enhances the diamond/Cu interfacial adhesion, as well as thermal conductivity. In this study, the optimum treatment temperature to form SiC on diamond to apply to SiC-coated diamond/Cu composite platings for improving the interfacial adhesion and thermal conductivity is investigated. The formation of SiC on the diamond surface was greatly affected by the treatment temperature, and the coverage of the SiC coating on the diamonds increased with treatment temperature. The formation of a more uniform SiC coating contributed to improved interfacial adhesion between the diamond and electrodeposited Cu matrix. The thermal conductivity of the SiC-coated diamond/Cu composite plating generally increased with an increase in temperature; however, excessive heat treatment at 1450°C decreased the thermal conductivity. The composite platings using SiC-coated diamond prepared at 1400°C showed a maximum thermal conductivity of 454 Wm−1K−1, which was higher than that of pure Cu platings (373 Wm−1K−1) and pristine diamond/Cu composite platings (375 Wm−1K−1).

DOI： 10.1080/09276440.2021.1937856

Nano ferric oxide adsorbents with self-acidification effect for efficient adsorption of Sb(V) 査読有り国際共著国際誌

Feng X., Yan R., Zhang Q., Wan Q., Hagio T., Ichino R., Kong L., Cao X., Li L.

Chemosphere 272 巻 2021年6月

The effect of bath pH on electrodeposition and corrosion properties of ternary Fe-W-Zn alloy platings 査読有り国際誌

Park Jae-Hyeok, Hagio Takeshi, Kamimoto Yuki, Ichino Ryoichi

JOURNAL OF SOLID STATE ELECTROCHEMISTRY 25 巻 ( 6 ) 頁： 1901 - 1913 2021年6月

担当区分：責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Journal of Solid State Electrochemistry

As a new trial to improve the corrosion resistance of the Fe-W alloy platings, Fe-W alloys incorporating a small amount of Zn, namely novel ternary Fe-W-Zn alloy platings, are prepared by constant current electrolysis using citrate-ammonia baths. In this study, the effects of bath pH on elemental composition, morphology, plating structure, and corrosion resistance of the electrodeposited ternary alloy platings are investigated. The W content of the electrodeposited alloys showed a maximum of 31.5 at.% at pH 8.0 and an inverse correlation was observed between the W content and current efficiency in the investigated pH range. The Zn content tended to decrease with increasing bath pH, and the structure of alloy platings gradually refined along with the increase in the amount of Zn incorporated into the Fe-W alloy. Potentiodynamic polarization test results reveal fine granular structured ternary Fe-W-Zn alloy prepared at pH 8.0, containing approximately 1.6 at.% of Zn, which showed distinctly enhanced corrosion resistance in a 1 M H2SO4 solution compared to binary Fe-W alloy and ternary alloys prepared at pH 6.0, 7.0, and 9.0. It has been found that the bath pH has a great influence on the elemental composition of the ternary alloys, which significantly affects the plating structure and corrosion resistance of the alloy platings.

DOI： 10.1007/s10008-021-04964-4

Band Gap Engineering toward Wavelength Tunable CsPbBr3 Nanocrystals for Achieving Rec. 2020 Displays 査読有り国際共著国際誌

Zhang Qinggang, Sun Xiaochuan, Zheng Weilin, Wan Qun, Liu Mingming, Liao Xinrong, Hagio Takeshi, Ichino Ryoichi, Kong Long, Wang Huamiao, Li Liang

CHEMISTRY OF MATERIALS 33 巻 ( 10 ) 頁： 3575 - 3584 2021年5月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Chemistry of Materials

For next-generation high-definition displays, the newly recommendation 2020 (Rec. 2020) standard calls for the emission wavelength of green emitters to be kept at 525-535 nm with narrow emission line width below 25 nm. All-inorganic lead halide perovskite CsPbBr3 nanocrystals (NCs) with sharp emission seem as the prefect one to match the call, however, it is a great challenge to tune their emission wavelength to the target window of 525-535 nm because of the intrinsic band gap of CsPbBr3. Herein, we report a facile strategy to prepare CsPbBr3 NCs with finely tunable emissions in the narrow range of 525-535 nm by establishing a CsPbBr3-Cs4PbBr6:Na Type II structure. The doping of the Na ions is the key factor to construct the Type II structure, which induces the formation of the Cs4PbBr6:Na phase and builds CsPbBr3-Cs4PbBr6:Na Type II structure, leading to the tunable emission wavelength of CsPbBr3 NCs. The as-synthesized CsPbBr3 NCs exhibit an ideal emission at 525-535 nm with a narrow emission line width of 23 nm and a high photoluminescence quantum yield (PLQY) of 85%. As a green downconverter, an ultrapure green backlight covers 97% of the Rec. 2020 standard in the CIE 1931 color space, representing the "greenest"backlight up to now.

DOI： 10.1021/acs.chemmater.1c00145

Progress in modifications of 3D graphene-based adsorbents for environmental applications 査読有り国際共著国際誌

Lin Y., Tian Y., Sun H., Hagio T.

Chemosphere 270 巻 2021年5月

Facile Hydrothermal Synthesis of EAB-Type Zeolite under Static Synthesis Conditions 査読有り国際共著国際誌

Hagio Takeshi, Park Jae-Hyeok, Lin Yan, Tian Yanqin, Hu Yun Hang, Li Xinling, Kamimoto Yuki, Ichino Ryoichi

CRYSTAL RESEARCH AND TECHNOLOGY 56 巻 ( 4 ) 頁： 2000163 2021年4月

担当区分：筆頭著者,　責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Crystal Research and Technology

Conventionally, EAB-type zeolites are crystallized by hydrothermal synthesis for many days under agitational synthesis conditions such as rotation or stirring. In the present study, EAB-type zeolite is obtained by hydrothermal synthesis within 12 h under static synthesis conditions for the first time. The effects of crystallization temperature, aging of the precursor sol, and addition of seed crystals are investigated. The results reveal that EAB-type zeolite can be obtained when using a precursor sol with short aging time followed by hydrothermal synthesis in a very narrow temperature range 110 °C−120 °C under static synthesis condition. Addition of seed crystals is found to suppress the formation of SOD-type zeolite, the primary phase at high hydrothermal synthesis temperatures, while it does not increase the crystallization rate of EAB-type zeolite. Furthermore, the crystallization behavior at 120 °C is examined by varying the synthesis time. EAB-type zeolite with invariably twinned plate-like morphology starts to crystallize between synthesis time of 3 to 6 h at 120 °C under the static synthesis condition.

DOI： 10.1002/crat.202000163

Synthesis of C-plane oriented hexagonal tungsten oxide membranes on tubular substrates and their acetic acid/water separation performances 査読有り国際共著国際誌

Kunishi H., Wada S., Kamimoto Y., Ichino R., Lin Y., Kong L., Li L., Hagio T.

Membranes 11 巻 ( 1 ) 頁： 1 - 17 2021年1月

Electrodeposition of Ni-W/CNT Composite Plating and Its Potential as Coating for PEMFC Bipolar Plate 査読有り国際誌

COATINGS 10 巻 ( 11 ) 頁： 1 - 14 2020年11月

担当区分：責任著者記述言語：日本語掲載種別：研究論文（学術雑誌）出版者・発行元：Coatings

In this study, Ni-W/carbon nanotube (CNT) composite platings are electrodeposited onto steel plate as a possible coating material for the polymer electrolyte membrane fuel cell (PEMFC) bipolar plate, which requires high corrosion resistance under acidic environment and low contact resistance. The dispersibility of CNT in the plating bath is improved by surface modification of CNT through hydrothermal treatment in mixed acid solution. The change in electrodeposition behavior of Ni-W plating by CNT addition is investigated by cathodic polarization measurement. The corrosion resistance under acidic environment is evaluated using 0.5M H2 SO4 solution and contact resistance of the composite platings is measured and compared with Ni and Ni-W plating. The surface modification of CNT through hydrothermal treatment is found to increase the CNT content in the Ni-W/CNT composite plating up to 0.33 mass.% and sufficient incorporation of hydrothermally treated CNT in Ni-W plating results in low contact resistance and enhanced corrosion resistance than pristine Ni-W plating.

DOI： 10.3390/coatings10111095

Surface-microporous graphene for CO2 adsorption 査読有り国際誌

Tian Yanqin, Lin Yan, Hagio Takeshi, Hu Yun Hang

CATALYSIS TODAY 356 巻頁： 514 - 518 2020年10月

Electrodeposition of a Novel Ternary Fe-W-Zn Alloy: Tuning Corrosion Properties of Fe-W Based Alloys by Zn Addition 査読有り国際誌

Park Jae-Hyeok, Hagio Takeshi, Kamimoto Yuki, Ichino Ryoichi

JOURNAL OF THE ELECTROCHEMICAL SOCIETY 167 巻 ( 13 ) 2020年10月

Rapid determination of iron concentration in wastewater using color band formation 査読有り国際誌

Imai Ryota, Kamimoto Yuki, Hagio Takeshi, Jung Yong-Jun, Ichino Ryoichi

SN APPLIED SCIENCES 2 巻 ( 9 ) 2020年8月

記述言語：日本語掲載種別：研究論文（学術雑誌）出版者・発行元：SN Applied Sciences

High concentrations of iron ions in water bodies cause odour and discolouration due to their precipitation. The total iron ion concentration is generally analysed on-site by forming coloured compounds and measuring colour intensity with spectrophotometric or visual analysis. In this work, we developed a detection tube as an alternative simple analytical method, where the total iron ion concentration is measured not by colour but by an objective parameter called the colour band length (CBL). Tiron was selected as the colouring agent since it oxidises divalent iron ions into a trivalent state and reacts with trivalent iron ions to form a 3:1 anion complex in alkaline media, giving a red colour. The coloured solution penetrates the detection tube by capillarity, and the colour band is formed by the entrapment of the hydrophobic ion pair of iron-tiron complex and quaternary ammonium ions of the adsorbent filled in the tube. The CBL was found to correlate well with the total iron ion concentration quantitatively under the optimized measurement condition, and 5 to 40 mg-FeL−1 solutions could be measured with good objectivity and precision.

DOI： 10.1007/s42452-020-03331-8

Improvement in corrosion resistance of ternary Zn-Fe-Mo plating by additional Mo-oxide coating 査読有り国際共著国際誌

Park Jae-Hyeok, Kosugi Daichi, Hagio Takeshi, Kamimoto Yuki, Ichino Ryoichi, Lee Myeong-Hoon

Surface and Coatings Technology 389 巻 2020年5月

Enhancement of corrosion resistance by lamination of Mg film on Zn-55Al-1.6Si-coated steel by physical vapor deposition 査読有り国際共著国際誌

Park Jae-Hyeok, Hagio Takeshi, Kamimoto Yuki, Ichino Ryoichi, Lee Myeong-Hoon

Surface and Coatings Technology 387 巻 2020年4月

Development of Synthetic Magnetic Zeolite Adsorbents and Application to Ammonium Ion Removal 査読有り国際共著国際誌

Kamimoto Yuki, Hagio Takeshi, Jung Yong-Jun, Ichino Ryoichi, Gil Kyungik

KSCE JOURNAL OF CIVIL ENGINEERING 2020年4月

Magnetic BEA-type zeolites: preparation by dry-gel conversion method and assessment of dye removal performance 査読有り国際共著国際誌

Phouthavong Vanpaseuth, Hiraiwa Masatake, Hagio Takeshi, Nijpanich Supinya, Chounlamany Vanseng, Nishihama Tatsuo, Kamimoto Yuki, Ichino Ryoichi

JOURNAL OF MATERIAL CYCLES AND WASTE MANAGEMENT 22 巻 ( 2 ) 頁： 375-382 2020年3月

Electrochemical behavior of tungsten carbide-cobalt alloy using molten hydroxide as electrolyte under low temperature 査読有り国際共著国際誌

Kamimoto Yuki, Kasuga Ren, Takeshita Kyohei, Hagio Takeshi, Kuroda Kensuke, Ichino Ryoichi, Deevanhxay Phengxay

JOURNAL OF MATERIAL CYCLES AND WASTE MANAGEMENT 22 巻 ( 2 ) 頁： 348-353 2020年3月

Nickel-carbon composite plating using a Watts nickel electroplating bath 国際共著国際誌

Kamimoto Yuki, Okura Shintaro, Hagio Takeshi, Wada Tatsuya, Tanaka Hidekazu, Hara Hideki, Deevanhxay Phengxay, Ichino Ryoichi

SN APPLIED SCIENCES 2 巻 ( 2 ) 2020年2月

記述言語：日本語掲載種別：研究論文（学術雑誌）出版者・発行元：SN Applied Sciences

Metal–carbon composite platings have potential applications in various fields. We previously reported the preparation of nickel–nanocarbon composite platings using a Wood’s bath. The maximum carbon content was 1.2 mass%, but the maximum current efficiency of plating was 12%. The present study focuses on improving the current efficiency of the electroplating process used to prepare nickel–carbon black composites in a Watts bath contained carbon black. The microstructure and carbon content in the nickel plating were evaluated. The current efficiency was greater than 90%, but the carbon content of the composite plating layer was approximately 0.6 mass%. The incorporation of carbon black particles into the plating layer was influenced by the adsorption of particles onto the cathode surface, the supply of particles to the surface, and the electrodeposition rate. The carbon content in the plating layer was highest near the cathode surface and decreased with increasing thickness of the plating layer. The grain size of electrodeposits with carbon black was larger than that of deposits without carbon black. The space between grains was increased with increasing grain size. The corrosion resistance was diminished, indicating that the boundary was the originating point of corrosion.

DOI： 10.1007/s42452-020-1991-1

Investigation on Strontium Adsorption Selectivity of Hydrothermally Synthesized Layered Sodium Titanates 査読有り国際誌

Kunishi Hiroto, Hagio Takeshi, Kamimoto Yuki, Ichino Ryoichi

SCIENCE OF ADVANCED MATERIALS 12 巻 ( 2 ) 頁： 186 - 190 2020年2月

Floating Adsorbent for Organic Removal Fabricated Through Crystallization of Silicalite-1 on Hollow Glass Microspheres 査読有り国際誌

Nijpanich Supinya, Hagio Takeshi, Kamimoto Yuki, Ichino Ryoichi

SCIENCE OF ADVANCED MATERIALS 12 巻 ( 2 ) 頁： 173 - 179 2020年2月

Development of magnesium-iron layered double hydroxide and application to nitrate removal 国際共著国際誌

Kamimoto Yuki, Okamoto Naoki, Hagio Takeshi, Yong-Jun Jung, Deevanhxay Phengxay, Ichino Ryoichi

SN APPLIED SCIENCES 1 巻 ( 11 ) 2019年11月

記述言語：日本語掲載種別：研究論文（学術雑誌）出版者・発行元：SN Applied Sciences

Nitrate is an important ion in agriculture and industry although it is known to cause eutrophication and affect human health. Removal of nitrogen by physicochemical treatment such as sedimentation and membrane separation remains difficult. The selectivity of commercial adsorbents for nitrate is among the lowest for anions, because the selectivity of an adsorbent as an ion exchange resin is based on the valence of the ion. Layered double hydroxide acts as an anion adsorbent, and the target anion adsorbs in the interlayer of cations. In this study, we focused on nitrate adsorption by magnesium-iron layered double hydroxide. The results indicate that the magnesium to iron ratio controlled the interlayer distance. The interlayer distance increased as the magnesium to iron ratio increased. The maximum adsorption capacity for nitrate of 1.80 mmol/g suggests the optimum magnesium to iron ratio is 3. The interlayer distance for a magnesium to iron ratio of 3 is similar in size to that of nitrate. The phosphate inhibition of nitrate adsorption suggests the formation of phosphate compounds on the adsorbent’s surface.

DOI： 10.1007/s42452-019-1240-7

Synthesis of MOR Zeolite/Magnetite Composite via Seed Assisted Method 査読有り国際共著国際誌

Hagio Takeshi, Nijpanich Supinya, Kunishi Hiroto, Yamaoka Keiichi, Phouthavong Vanpaseuth, Kamimoto Yuki, Ichino Ryoichi, Iwai Kazuhiko

JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY 19 巻 ( 10 ) 頁： 6841-6848 2019年10月

Preparation of a floating photocatalyst via electroless Ni-P-TiO₂ composite plating on polypropylene balls for wastewater treatment 査読有り国際誌

Nijpanich Supinya, Hagio Takeshi, Kamimoto Yuki, Ichino Ryoichi

Journal of Water and Environment Technology 17 巻 ( 3 ) 頁： 131-140 - 140 2019年

Electrodeposition of rare-earth elements from neodymium magnets using molten salt electrolysis 査読有り国際誌

Kamimoto Y., Itoh T., Yoshimura G., Kuroda K., Hagio T., Ichino R.

JOURNAL OF MATERIAL CYCLES AND WASTE MANAGEMENT 20 巻 ( 4 ) 頁： 1918-1922 2018年10月

Development of Metal-Carbon Black Composite Plating with Wood's Bath 査読有り国際共著国際誌

Kamimoto Yuki, Ohkura Shintaro, Tanaka Hidekazu, Hara Hideki, Hagio Takeshi, Deevanhxay Phengxay, Ichino Ryoichi

NANOSCIENCE AND NANOTECHNOLOGY LETTERS 10 巻 ( 5-6 ) 頁： 805-808 - 808 2018年5月

Seed-Assisted Synthesis of Magnetic Faujasite-Type Zeolite and Its Adsorption Performance 査読有り国際誌

Hagio Takeshi, Kunishi Hiroto, Yamaoka Keiichi, Kamimoto Yuki, Ichino Ryoichi

NANOSCIENCE AND NANOTECHNOLOGY LETTERS 10 巻 ( 5-6 ) 頁： 862-867 - 867 2018年5月

Synthesis of Magnetic Activated Carbon Based on a Magnetite/Butyl Glycidyl Ether-Diluted Bisphenol A/Diethylenetriamine Epoxy Resin System 査読有り国際誌

Nijpanich Supinya, Morihashi Ryo, Hagio Takeshi, Kamimoto Yuki, Ichino Ryoichi

NANOSCIENCE AND NANOTECHNOLOGY LETTERS 10 巻 ( 5-6 ) 頁： 843-848 - 848 2018年5月

Electrodeposition of Copper/Carbonous Nanomaterial Composite Coatings for Heat-Dissipation Materials 査読有り国際誌

Goto Yasuki, Kamebuchi Yota, Hagio Takeshi, Kamimoto Yuki, Ichino Ryoichi, Bessho Takeshi

COATINGS 8 巻 ( 1 ) 2018年1月

Effect of the Addition of Molybdenum on the Structure and Corrosion Resistance of Zinc-Iron Plating 査読有り国際誌

Kosugi Daichi, Hagio Takeshi, Kamimoto Yuki, Ichino Ryoichi

COATINGS 7 巻 ( 12 ) 2017年12月

Phosphorus removal and magnetic separation using magnetic schwertmannite 査読有り国際共著国際誌

Kamimoto Yuki, Yamauchi Kazushige, Hagio Takeshi, Ichino Ryoichi, Min Kyung Sok, Kwon Koo Ho, Kim Ye Jin, Jung Yong Jun

DESALINATION AND WATER TREATMENT 63 巻頁： 463-468 2017年2月

Thermoelectric properties of crystal aligned higher manganese silicide fabricated by solidification under magnetic field 査読有り国際誌

K. Yamauchi, T. Hagio, T. Mitsuo, T. Itoh and K. Iwai

Japanese Journal of Applied Physics 54 巻 ( 11 ) 2015年11月

Electrochemical leaching of tungsten from hard metal alloy using molten sodium hydroxide 査読有り国際誌

Y. Kamimoto, M. Kamiya, R. Kasuga, T. Hagio, K. Kuroda and R. Ichino

Materials Transactions 56 巻 ( 5 ) 頁： 733 - 737 2015年

Beta tricalcium phosphate ceramics with controlled crystal orientation fabricated by application of external magnetic field during the slip casting process 査読有り国際誌

T. Hagio, K. Yamauchi, T. Kohama, T. Matsuzaki, K. Iwai

Materials Science and Engineering C 33 巻 ( 5 ) 頁： 2967 - 2970 2013年7月

Difference in bioactivity, initial cell attachment and cell morphology observed on the surface of hydroxyapatite ceramics with controlled orientation 査読有り国際誌

Hagio Takeshi, Tanase Tomohiko, Akiyama Jun, Iwai Kazuhiko, Asai Shigeo

Materials Transactions 50 巻 ( 4 ) 頁： 734 - 739 2009年4月

Different properties exhibited on the two typical crystal faces of hydroxyapatite in a simulated body environment 査読有り国際誌

Hagio Takeshi, Tanase Tomohiko, Akiyama Jun, Umino Masanori, Iwai Kazuhiko, Asai Shigeo

Journal of Physics: Conference Series 156 巻 2009年

Formation and biological affinity evaluation of crystallographically aligned hydroxyapatite 査読有り国際誌

Hagio Takeshi, Tanase Tomohiko, Akiyama Jun, Iwai Kazuhiko, Asai Shigeo

JOURNAL OF THE CERAMIC SOCIETY OF JAPAN 116 巻 ( 1349 ) 頁： 79 - 82 2008年1月

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