研究者詳細 - 日比野　高士

論文 - 日比野　高士

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Cathodes for High-Temperature PEM Fuel Cells Based on a Si0.97Al0.03C Promoter and a Sn0.95In0.05P2O7 Ionomer 査読有り

Harada T., Jin Y. C., Heo P., Hibino T.

FUEL CELLS 10 巻 ( 5 ) 頁： 798 - 803 2010年10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：Fuel Cells

This paper presents a promising approach to reduce the quantity of Pt required in cathodes for high-temperature proton exchange membrane (PEM) fuel cells. Based on preliminary experiments, thermally stable Si 0.97Al0.03C and Sn0.95In0.05P 2O7 were selected as promoter and ionomer, respectively. Si0.97Al0.03C particles (∼40 nm) and Sn 0.95In0.05P2O7 particles (∼45 nm) were successfully produced on a carbon support. Pt particles (∼9 nm) were selectively impregnated in the vicinity of the ionomer. Polarisation measurements revealed that the Pt-Sn0.95In0.05P 2O7-Si0.97Al0.03C/C cathode exhibited much higher oxygen reduction reaction (ORR) activity than that observed for a pure Pt/C cathode, due to the enhanced dissociative oxygen adsorption on the Si0.97Al0.03C particles and the increased number of reaction sites for the ORR provided by the Sn 0.95In0.05P2O7 particles. Fuel cell operation tests demonstrated that a Pt-Sn0.95In0.05P 2O7-Si0.97Al0.03C/C cathode with a low Pt loading of 0.1 mg cm-2 provides better cell performance than a Pt/C cathode with a Pt loading of 1.0 mg cm-2. © 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

DOI： 10.1002/fuce.200900162

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Proton conduction in metal pyrophosphates (MP2O7) at intermediate temperatures 査読有り

Yongcheng Jin, Yanbai Shen, Takashi Hibino

Journal of Materials Chemistry 20 巻頁： 6214-6217 2010年8月

Low-temperature hydrocarbon combustion over proton conductor/metal-mixed catalysts 査読有り

Tsuneyama Kota, Tetanishi Shinya, Hibino Takashi, Nagao Satoshi, Hirata Hirohito, Matsumoto Shin-ichi

JOURNAL OF CATALYSIS 273 巻 ( 1 ) 頁： 59 - 65 2010年7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：Journal of Catalysis

Catalytic combustion of hydrocarbons is a highly active field of research, particularly in relation to the reduction of pollutant emissions from automobiles. In this study, we report on hydrocarbon oxidation at the internal interfaces of a mixed catalyst consisting of Sn0.9In 0.1P2O7 and Pt powders. In a gaseous mixture of propane, H2O, and O2, the H2O dissociates into protons, electrons and active oxygen species at anodic interface sites, leading to oxidation of the hydrocarbon to CO2. On the other hand, O 2 reacts with protons and electrons to form H2O at cathodic interface sites. As a consequence, local electrochemical cells are formed at the interfaces, and undergo self-discharge. It was shown that the mixed catalyst had a high turnover frequency for Pt, yielding high catalytic activity for Pt contents of as low as 0.1 wt% and an initiation temperature for hydrocarbon oxidation of 150 °C. © 2010 Elsevier Inc.

DOI： 10.1016/j.jcat.2010.04.022

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Low-temperature hydrocarbon combustion over proton conductor/metal-mixed catalysts 査読有り

Kota Tsuneyama, Shinya Teranishi, Takashi Hibino, Satoshi Nagao, Hirohito Hirata, Shin-ichi Matsumoto

Journal of Catalysis 273 巻頁： 59-65 2010年7月

Direct oxidation of methane to methanol over proton conductor/metal mixed catalysts 査読有り

Lee Byungik, Sakamoto Yosuke, Hirabayashi Daisuke, Suzuki Kenzi, Hibino Takashi

JOURNAL OF CATALYSIS 271 巻 ( 2 ) 頁： 195 - 200 2010年5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：Journal of Catalysis

The intermediate-temperature and low-pressure production of methanol from methane in a one-pass process was investigated using a micro- or nanosized electrocatalyst system. The powdered catalyst was prepared by mixing proton-conducting Sn0.9In0.1P2O7 particles with high-activity Pd-Au-Cu/C particles to provide numerous electrolyte-electrode interfaces as reaction sites for methane oxidation. For a feed mixture of H2O, O2, and methane, a local electrochemical cell can be formed at the electrode-electrolyte interface: H2O → 1/2O2 + 2H+ + 2e- at the anode site; O2 + CH4 + 2H+ + 2e- → CH3OH + H2O at the cathode site. In addition, the electrode also functions as a lead wire that short-circuits the cell. Therefore, the overall reaction can be expected to be CH4 + 1/2O2 → CH3OH. The series of reactions successfully resulted in reduction in the temperature for initiation of methane oxidation to 250 °C and increased the methanol yield while maintaining a very high selectivity toward methanol for temperatures up to 400 °C. © 2010 Elsevier Inc. All rights reserved.

DOI： 10.1016/j.jcat.2010.01.011

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Direct oxidation of methane to methanol over proton conductor/metal mixed catalysts 査読有り

Byung Ik Lee, Yosuke Sakamoto, Daisuke Hirabayashi, Kenzi Suzuki, Takashi Hibino

Journal of Catalysis 271 巻頁： 195-200 2010年5月

Alumina substrate-supported electrochemical device for potential application as a diesel particulate matter sensor 査読有り

Shen Yanbai, Takeuchi Takashi, Teranishi Shinya, Hibino Takashi

SENSORS AND ACTUATORS B-CHEMICAL 145 巻 ( 2 ) 頁： 708 - 712 2010年3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：Sensors and Actuators, B: Chemical

The carbon oxidation activity and sensing performance of an alumina substrate-supported sensor comprised of Sn0.9In0.1P2O7 as a proton conductor and Pt as an electrocatalyst were investigated. Electrochemically formed active oxygen species exhibited high activity for carbon oxidation, where the current efficiency was estimated from the four-electron reaction (C + 2H2O → CO2 + 4H+ + 4e-) and reached approximately 90%. An operating temperature of 225 °C was found to be the most effective to achieve the highest possible electrochemical carbon oxidation and the lowest possible non-electrochemical carbon oxidation. When carbon introduced to the Sn0.9In0.1P2O7-Pt interface was oxidized by active oxygen, a large potential jump was observed due to a significant increase in the polarization resistance, which was strongly dependent on the carbon content in the working electrode. Two types of carbon sensors, amperometric and potentiometric, were tested in a feed mixture of 3 vol% water vapor and 10 vol% O2. In the case of the amperometric sensor, the current increased linearly with increasing carbon content, which enabled the determination of a wide range of carbon content from the current signal. In the case of the potentiometric sensor, a threshold quantity of carbon could be recognized by selection of the current and subsequent monitoring of the sudden potential increase. © 2010 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.snb.2010.01.030

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Alumina substrate-supported electrochemical device for potential application as a diesel particulate matter sensor 査読有り

Yanbai Shen, Takashi Takeuchi, Shinya Teranishi, Takashi Hibino

Sensors and Actuators B: Chemical 145 巻頁： 708-712 2010年3月

High-temperature low-humidity proton exchange membrane based on an inorganic-organic hybrid structure 査読有り

Yongcheng Jin, keisuke Fujiwara, Takashi Hibino

Electrochemical and Solid-State Letters 13 巻 ( 2 ) 頁： B8-B10 2010年2月

Development and application of SnP2O7-based proton conductors to intermediate-temperature fuel cells 招待有り査読有り

Yongcheng Jin, Byung Ik Lee, Takashi Hibino

Journal of the Japan Petroleum Institute 53 巻 ( 1 ) 頁： 12-23 2010年1月

Development and Application of SnP2O7-based Proton Conductors to Intermediate-temperature Fuel Cells 査読有り

Jin Yongcheng, Lee Byungik, Hibino Takashi

JOURNAL OF THE JAPAN PETROLEUM INSTITUTE 53 巻 ( 1 ) 頁： 12 - 23 2010年1月

総説：燃料電池による排ガスからのエネルギー回収

日比野高士，内山靖之，内山直樹

セラミックス 45 巻頁： 548-552 2010年

High Temperature, Low Humidity Proton Exchange Membrane Based on an Inorganic-Organic Hybrid Structure 査読有り

Jin Yongcheng, Fujiwara Keisuke, Hibino Takashi

ELECTROCHEMICAL AND SOLID STATE LETTERS 13 巻 ( 2 ) 頁： B8 - B10 2010年

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：Electrochemical and Solid-State Letters

A high temperature and low humidity composite membrane consisting of Sn0.95 Al0.05 P2 O7 and sulfonated polystyrene- b -poly(ethylene/butylene)- b -polystyrene (sSEBS) as inorganic and organic materials, respectively, was prepared and characterized. A homogeneous distribution of the Sn0.95 Al0.05 P2 O 7 particles in the matrix was accomplished in the thickness range of 25-80 μm, providing an elongation at break above 400%, which is approximately two times higher than that for Nafion. Moreover, moderate proton conductivities of sSEBS improved proton transfer between the Sn0.95 Al 0.05 P2 O7 particles in the matrix, resulting in a proton conductivity of approximately 0.01 S cm-1 at 130°C without any humidification, which is 3 or more orders of magnitude higher than that for Nafion under the same conditions. © 2009 The Electrochemical Society.

DOI： 10.1149/1.3267848

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Partially Proton-Exchanged WP2O7 with High Conductivity at Intermediate Temperatures 査読有り

Jin Y. C., Yang L., Nishida M., Kanematsu W., Hibino T.

ELECTROCHEMICAL AND SOLID STATE LETTERS 13 巻 ( 11 ) 頁： B123 - B126 2010年

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：Electrochemical and Solid-State Letters

Proton conduction is reported in partially proton-exchanged WP2 O7 at intermediate temperatures. Electrochemical measurements demonstrated that proton conduction occurs in this material. Proton magic angle spinning nuclear magnetic resonance and Fourier transform IR analyses revealed that the ion-exchanged protons interact with the lattice oxide ions in WP 2 O7 to form hydrogen bonds. The H/D isotope effect suggests that proton conduction in this material is based on the hopping mechanism. Consequently, the electrical conductivity of this material reached 1.1× 10-3 S cm-1 at 250°C and 1.7× 10 -2 S cm-1 at 500°C. © 2010 The Electrochemical Society.

DOI： 10.1149/1.3485076

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Proton conduction in metal pyrophosphates (MP2O7) at intermediate temperatures 査読有り

Jin Yongcheng, Shen Yanbai, Hibino Takashi

JOURNAL OF MATERIALS CHEMISTRY 20 巻 ( 30 ) 頁： 6214 - 6217 2010年

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：Journal of Materials Chemistry

Intermediate-temperature fuel cells have received much recent attention as next generation energy sources. In particular, current efforts are devoted to developing proton conductors that operate at 120°C or more and at low relative humidity. Proton conduction in several metal pyrophosphates (MP 2O7, M = Sn, Ti, Si, Ge, Ce, and Zr) that have the potential to meet the demands for intermediate-temperature fuel cell applications are reviewed with an emphasis on the material aspects. © 2010 The Royal Society of Chemistry.

DOI： 10.1039/b924188d

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Proton-conducting thin film grown on Yttria-stabilized Zirconia surface for Ammonia gas sensing technologies 査読有り

Shinya Teranishi, Kyohei Kondo, Masakazu Nishida, Wataru Kanematsu, Takashi Hibino

Electrochemical and Solid-State Letters 12 巻 ( 9 ) 頁： J73-J76 2009年9月

Proton conductivity and solid acidity of Mg-, In-, and Al-doped SnP2O7 査読有り

Kouji Genzaki, Pilwon Heo, Mitsuru Sano, Takashi Hibino

Journal of the Electrochemical Society 156 巻 ( 7 ) 頁： B806-B810 2009年7月

Selective electrochemical oxidation of carbon by active oxygen for potential application as a sensor for diesel particulates 査読有り

Teranishi Shinya, Kondo Kyohei, Tsuge Akihito, Hibino Takashi

SENSORS AND ACTUATORS B-CHEMICAL 140 巻 ( 1 ) 頁： 170 - 175 2009年6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：Sensors and Actuators, B: Chemical

The formation of active oxygen by electrochemical oxidation of H2O vapor, coupled with carbon detection using those oxygen species, has been investigated by utilizing Sn0.9In0.1P2O7 as a proton conductor and Pt as an electrocatalyst. The H2O vapor was dissociated into protons and electrons at a Pt-carbon working electrode, which produced active oxygen on the carbon surface. This oxygen species showed high activity for carbon oxidation at temperatures of 50 °C or higher, where CO2 formation increased with temperature and reached the theoretical value calculated from the four-electron reaction (C + H2O → CO2 + 4H+ + 4e-) at 200 °C. When the formation rate of active oxygen was greater than the oxidation rate of carbon at the working electrode, the electrode potential increased rapidly due to a significant increase in polarization resistance. The timing of the potential jump was strongly dependent on both the carbon content in the working electrode and the current to the working electrode, which provides information on the quantity of carbon. In addition, little interference was encountered in sensing for carbon at 1000 ppm CO and 1000 ppm C3H8 in the sample gas. The high selectivity toward carbon was based on different mechanisms for CO and C3H8; almost all of the CO was catalytically oxidized to CO2 before reacting with active oxygen, while C3H8 experienced little reaction with active oxygen. These results demonstrate that the present sensor sensitively and selectively detects carbon while self-regenerating. © 2009 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.snb.2009.04.044

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*Selective electrochemical oxidation of carbon by active oxygen for potential application as a sensor for diesel particulates 査読有り

Shinya Teranishi, Kyohei Kondo, Akihito Tsuge, Takashi Hibino

Sensors and Actuators B: Chemical 140 巻頁： 170-175 2009年6月

Nanostructured Pt-Sn1-xInxP2O7 cathodes for high-temrerature proton exchange membrane fuel cells 査読有り

Pilwon Heo, Toshihiko Harada, Takashi Hibino

Electrochemical and Solid State Letters 12 巻 ( 1 ) 頁： B1-B4 2009年1月

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