Faculty Profiles - HIBINO, Takashi

Papers - HIBINO, Takashi

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総説：電極触媒活性の精密制御に基づいたガスセンシング技術の開発と各種デバイスへの応用展開

日比野高士

Vol. 25 page： 38-40 2009

Nanostructured Pt-Sn(1-x)In(x)P(2)O(7) Cathodes for High-Temperature Proton Exchange Membrane Fuel Cells Reviewed

Heo Pilwon, Harada Toshihiko, Hibino Takashi

ELECTROCHEMICAL AND SOLID STATE LETTERS Vol. 12 ( 1 ) page： B1 - B4 2009

Language：Japanese Publishing type：Research paper (scientific journal) Publisher：Electrochemical and Solid-State Letters

Nanosized proton-conducting Sn0.95 In0.05 P2 O7 ionomers were grown on carbon supports by the coprecipitation of tin and indium chlorides with excess ammonia water and subsequent solid-state reaction with phosphoric acid. The resulting homogeneous networks of Sn0.95 In0.05 P2 O7 ionomers enhanced the activity of a Pt catalyst for the oxygen reduction reaction in the temperature range of 150-250°C. In addition, the Pt catalyst showed high corrosion resistance in the cathode environment while maintaining high performance levels. A comparison of the cathode performance between Sn0.95 In0.05 P2 O7 and H3 P O4 ionomers further demonstrated that the Sn0.95 In0.05 P2 O7 nanoparticles are promising candidates for cathode ionomer materials at high temperatures. © 2008 The Electrochemical Society.

DOI： 10.1149/1.3006328

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Proton Conductivity and Solid Acidity of Mg-, In-, and Al-Doped SnP2O7 Reviewed

Genzaki Kouji, Heo Pilwon, Sano Mitsuru, Hibino Takashi

JOURNAL OF THE ELECTROCHEMICAL SOCIETY Vol. 156 ( 7 ) page： B806 - B810 2009

Language：Japanese Publishing type：Research paper (scientific journal) Publisher：Journal of the Electrochemical Society

Mg-, In-, and Al-doped SnP2 O7 were synthesized, and their potential as electrolytes for fuel cells was evaluated in terms of their performance and durability. The overall conductivity of Mg-doped SnP2 O7 increased with increasing Mg2+ content and reached a maximum at 10 mol %. However, this was smaller than that obtained for doping with 10 mol % In3+ and 5 mol % Al3+, especially at temperatures below 300°C. This result was interpreted to be a consequence of lower proton mobility rather than of smaller proton concentration in Mg-doped SnP2 O7, probably due to the electrostatic restriction by Mg2+ against proton transport. Moreover, to investigate the influence of the Mg2+ doping on the fuel-cell properties, fuel-cell tests were conducted using Sn0.9 Mg0.1 P2 O7, Sn0.9 In0.1 P2 O7, and Sn0.95 Al0.05 P2 O7 as electrolytes at a temperature of 150°C. Compared with Sn0.9 In0.1 P2 O7 and Sn0.95 Al0.05 P2 O7 cells, the Sn0.9 Mg0.1 P2 O7 cell showed a somewhat higher Ohmic resistance but exhibited a comparable polarization resistance, which is the main component of the total electrical resistance. More importantly, the Mg2+ doping led to an improved stability of the Pt catalyst and carbon support at high potentials. This beneficial effect was attributed to a large reduction in the acidity of SnP2 O7 resulting from the basicity of MgO. © 2009 The Electrochemical Society.

DOI： 10.1149/1.3123219

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Proton-Conducting Thin Film Grown on Yttria-Stabilized Zirconia Surface for Ammonia Gas Sensing Technologies Reviewed

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

ELECTROCHEMICAL AND SOLID STATE LETTERS Vol. 12 ( 9 ) page： J73 - J76 2009

Language：Japanese Publishing type：Research paper (scientific journal) Publisher：Electrochemical and Solid-State Letters

We demonstrate an approach to impart both proton conduction and solid acidity to the surface of yttria-stabilized zirconia (YSZ). By reacting a YSZ substrate with liquid H3PO4 at 500°C, a thin Zr 1-xYx P2O7 film is grown on the substrate, which shows proton conductivity dependence on humidity and strong acid sites interacting with basic ammonia gas. This technique can be applied to gas sensor devices, yielding a remarkably sensitive and selective response to low concentrations (parts per million) of ammonia. Another important achievement of this technique is the realization of sensing properties in spite of using a conventional Pt electrode. © 2009 The Electrochemical Society.

DOI： 10.1149/1.3156836

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Nano-sized electrochemical reactors for selective NOx reduction Reviewed

Shinya Teranishi, Akihito Tuge, Atsuko Tomita, Mitsuru Sano, Takashi Hibino

Electrochemical and Solid-State Letters Vol. 11 ( 10 ) page： P9-P12 2008.10

A single-chamber SOFC stack:energy recovery from engin exhaust Reviewed

Masahiro Nagao, Masaya Yano, Kohsuke Okamoto, Atsuko Tamita, Yasuyuki Uchiyama, Naoki Uchiyama, Takashi Hibino

Fuel Cells Vol. 08 ( 5 ) page： 322-329 2008.10

A Single-Chamber SOFC Stack: Energy Recovery from Engine Exhaust Reviewed

Nagao M., Yano M., Okamoto K., Tomita A., Uchiyama Y., Uchiyama N., Hibino T.

FUEL CELLS Vol. 8 ( 5 ) page： 322 - 329 2008.10

Language：Japanese Publishing type：Research paper (scientific journal) Publisher：Fuel Cells

The feasibility of applying single-chamber solid oxide fuel cells (SC-SOFCs) to power generators for exhaust energy recovery was investigated using both model and actual exhaust gases. In the experiments with model exhaust gases, a single cell, Ni-Ce0.8Sm0.2O1.9/YSZ/ La0.8Sr0.2MnO3, was operated in a mixture of gases containing ppm levels of CH4, C2H6, C3H3, C4H10and O2. The cell performance was considerably affected by the molar ratio of total hydrocarbons to O2, the operating temperature and the gas flow rate. The optimal operating conditions of the SC-SOFC were found to be similar to those found in actual exhaust from gasoline engines. Thermal and mechanical loading performance tests demonstrated high tolerance towards thermal cycling and breakage of the electrolyte. Performance tests with and without a gas separator suggested that there is no requirement for a gas separator in an actual exhaust. In the experiments with actual exhaust gases, a 12-cell stack was installed to a 250-cm3 engine. The open circuit voltages (OCVs) were between 5 and 8 V and independent of the number of revolutions, but were lower than the values expected from the model exhaust results. This was considered to be due to the deviation of the actual exhaust gases from the model gases. Nevertheless, the stack performance was reproducible and stable in the range from 1,500 to 5,500 rpm. The resultant peak power reached above 1 W at 4,500 rpm. © 2008 WILEY-VCH Verlag GmbH & Co. KGaA.

DOI： 10.1002/fuce.200800017

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De-NOx reactor and NOx sensor using In3+-doped SnP2O7 with PtRhBa/C electrode Reviewed

Nagao Masahiro, Yoshii Takeshi, Namekata Yousuke, Teranishi Shinya, Sano Mitsuru, Tomita Atsuko, Hibino Takashi

SOLID STATE IONICS Vol. 179 ( 27-32 ) page： 1655 - 1661 2008.9

Language：Japanese Publishing type：Research paper (scientific journal) Publisher：Solid State Ionics

An electrochemical cell using an In3+-doped SnP2O7 proton conductor as the electrolyte exhibited comparable NO reduction and sensing properties at around 250 °C. NO was reduced to N2 most effectively when using a PtRhBa/C cathode by applying current to the cell. High electrocatalytic activity was maintained even in the presence of CO2 and H2O. PtRhBa/C was also found to be the most effective electrode material for NOx sensing. The sensor exhibited electromotive force (EMF) response towards the positive direction with increasing NO and NO2 concentrations. The polarization curves of NO/NO2 and water vapor indicated that the sensing mechanism is based on the mixed potential. The effects of added Rh and Ba to the Pt/C electrode were explained in terms of selective reduction and adsorption of NO/NO2 over the electrode surface, respectively. © 2008 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.ssi.2008.03.033

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Pt-free intermediate-temperature fuel cells Reviewed

Heo Pilwon, Shibata Hidetaka, Nagao Masahiro, Hibino Takashi

SOLID STATE IONICS Vol. 179 ( 27-32 ) page： 1446 - 1449 2008.9

Language：Japanese Publishing type：Research paper (scientific journal) Publisher：Solid State Ionics

Pt-free fuel cells were investigated using a proton-conducting Sn0.9In0.1P2O7 electrolyte at intermediate temperatures between 150 and 300 °C. Transition metal oxides were applied as non Pt cathode catalysts. A ZrO2/C catalyst showed the highest catalytic activity for the oxygen reduction reaction among the metal oxides tested. The catalytic activity of ZrO2/C was further improved by optimizing the heat-treatment temperature for ZrO2/C. XRD measurements revealed that the high catalytic activity was attributed to the crystal structure of tetragonal ZrO2. Finally, we evaluated performance of a Pt-free fuel cell using the ZrO2/C cathode with a Mo2C-ZrO2/C anode that shows Pt-like behavior in reducing atmospheres. Reasonable performance was achieved by operating the Pt-free fuel cell at intermediate temperatures above 200 °C. © 2008 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.ssi.2007.12.090

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A proton-conducting fuel cell operating with hydrocarbon fuels Reviewed

Pilwon Heo, Kenichi Ito, Atsuko Tomita, Takashi Hibino

Angewandte Chemie-international edition Vol. 120 page： 7959-7962 2008.9

De-NOx reactor and Nox sensor using In3+-doped SnP2O7 with PtRhBa/c electrode Reviewed

Masahiro Nagao, Takeshi Yoshii, Yousuke Namekata, Shinya Teranishi, Mitsuru Sano, Atsuko Tomita, Takashi Hibino

Solid State Ionics Vol. 179 page： 1655-1661 2008.9

Pt-free intermediate-temperature fuel cells Reviewed

Pilwon Heo, Hidetaka Sibata, Masahiro Nagao, Takashi Hibino

Solid State Ionics Vol. 179 page： 1446-1449 2008.9

Proton conduction in Sn0.95Al0.05P2O7-PBI-PTFE composite membrane Reviewed

Pilwon Heo, Norikazu Kajiyama, Kazuyo Kobayashi, Masahiro Nagao, Mitsuru Sano, Takashi Hibino

Electrochemical and Solid State Letters Vol. 11 ( 6 ) page： B91-B95 2008.6

Blocking of electronic current through a Ce0.9Gd0.1O1.95 electrolyte film by growth of a thin BaCe1-xGdxO3-alpha layer Reviewed

Atsuko Tomita, Yuki Tachi, Takashi Hibino

Electrochemical and Solid State Letters Vol. 11 ( 5 ) page： B68-B70 2008.5

*A singie-chamber SOFC stack operating in engine exhaust Reviewed

Masaya Yano, Masahiro Nagao, Kohsuke Okamoto, Atsuko Tomita, Yasuyuki Uchiyama, Naoki Uchiyama, Takashi Hibino

Electrochemical and Solid-State Letters Vol. 11 ( 3 ) page： B29-B33 2008.3

Direct oxidation of methane to methanol at low temperature and pressure in an electrochemical fuel cell Reviewed

Atsuko Tomita, Junya Nakajima, Takashi Hibino

Angewandte Chemie-international edition Vol. 47 page： 1462-1464 2008.1

Direct dimethyl ether fuel cella at intermediate temperatures Reviewed

Pilwon Heo, Masahiro Nagao, Mitsuru Sano, Takashi Hibino

Journal of The Electrochemical Society Vol. 155 ( 1 ) page： B92-B95 2008.1

A proton-conducting fuel cell operating with hydrocarbon fuels Reviewed

Heo Pilwon, Ito Kenichi, Tomita Atsuko, Hibino Takashi

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Vol. 47 ( 41 ) page： 7841 - 7844 2008

Language：Japanese Publishing type：Research paper (scientific journal) Publisher：Angewandte Chemie - International Edition

Low temperature, high voltage! Direct oxidation of hydrocarbon fuels, including methane, ethane, propane, and butane, occurs over Pt-free anodes in a proton-conducting fuel cell in the temperature range 100-300°C. A Mo 2C-ZrO2/C anode (30 mg Mo2C-ZrO2 per cm2) yields power densities equal to those obtained from Pt/C anodes (1-7 mg Pt per cm2) and generates higher open-circuit voltages than the Pt/C anodes. (Figure Presented) © 2008 Wiley-VCH Verlag GmbH & Co. KGaA.

DOI： 10.1002/anie.200801667

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Direct oxidation of methane to methanol at low temperature and pressure in an electrochemical fuel cell Reviewed

Tomita Atsitko, Nakajima Junya, Hibino Takashi

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Vol. 47 ( 8 ) page： 1462 - 1464 2008

Language：Japanese Publishing type：Research paper (scientific journal) Publisher：Angewandte Chemie - International Edition

(Chemical Equation Presented) Fuel for thought? The direct oxidation of methane to methanol occurs at atmospheric pressure between 50 and 250°C in a fuel-cell-type reactor (see picture). The efficiency of the electrochemical activation of oxygen is higher than that for the catalytic activation of oxygen. © 2008 Wiley-VCH Verlag GmbH & Co. KGaA.

DOI： 10.1002/anie.200703928

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Direct dimethyl ether fuel cells at intermediate temperatures Reviewed

Heo Pilwon, Nagao Masahiro, Sano Mitsuru, Hibino Takashi

JOURNAL OF THE ELECTROCHEMICAL SOCIETY Vol. 155 ( 1 ) page： B92 - B95 2008

Language：Japanese Publishing type：Research paper (scientific journal) Publisher：Journal of the Electrochemical Society

Direct dimethyl ether fuel cells (DDMEFCs) were investigated using proton-conducting Sn0.9 In0.1 P2 O7 as an electrolyte at intermediate temperatures between 150 and 300°C. Fuel cell operation at intermediate temperatures allowed a PtC anode to achieve excellent CO tolerance and high catalytic activity for the anode reaction of DME. The catalytic activity of the PtC anode was further improved by the addition of Ru to Pt, especially at elevated temperatures. The anodic overpotential and anode product measurements revealed that the H2 produced by the reforming reaction of DME was electrochemically oxidized at the PtRuC anode, which proceeded in parallel with the direct oxidation reaction of DME. As a result, DDMEFCs with the PtRuC anode achieved a peak power density of 31, 52, and 78 mW cm-2 at 200, 250, and 300°C, respectively. © 2007 The Electrochemical Society.

DOI： 10.1149/1.2803509

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Papers - HIBINO, Takashi