研究者詳細 - 日比野　高士

論文 - 日比野　高士

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Erratum: Room-temperature proton transport and its effect on thermopower in a solid ionic semiconductor, TTFCOONH<inf>4</inf> (Journal of Materials Chemistry A (2013) 1 (5089-5096) (DOI:10.1039/C3TA00011G)) 査読有り

Kobayashi Y., Fujii T., Terasaki I., Kino H., Jin Y., Hibino T., Kobayashi T., Nishibori E., Sawa H., Yoshikawa H., Terauchi T., Sumi S.

Journal of Materials Chemistry A 1 巻 ( 48 ) 2013年12月

Oxygen reduction reaction over nitrogen-doped graphene oxide cathodes in acid and alkaline fuel cells at intermediate temperatures 査読有り

Hibino Takashi, Kobayashi Kazuyo, Heo Pilwon

ELECTROCHIMICA ACTA 112 巻頁： 82 - 89 2013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：Electrochimica Acta

Graphene oxides with various nitrogen contents were prepared by annealing them in an NH3 flow between 350 and 850 C, and their electrocatalytic properties toward the oxygen reduction reaction (ORR) in acid and alkaline fuel cells at intermediate temperatures were investigated. In both acid and alkaline fuel cells, graphene oxide treated with NH3 at 700 C for 1 h was the most active cathode at operating temperatures between 75 and 200 C, where the ORR activity was enhanced by an increase in the operating temperature. This cathode also exhibited high chemical and thermal stability toward the ORR. X-ray photoelectron and Raman spectroscopic measurements of the nitrogen-doped graphene oxides indicated that the pyridinic nitrogen introduced disordered edge planes into the graphene structure. BET analysis also revealed that the surface area of graphene oxide was increased by the exposure of such edge planes. These observations lead to the assumption that the defects introduced by pyridinic nitrogen act as active sites for the ORR. Considering the similarity in ORR activity between the acid and alkaline fuel cells, dissociative adsorption of O2 at the active site is a rate-determining step. © 2013 Elsevier Ltd. All rights reserved.

DOI： 10.1016/j.electacta.2013.08.101

Organometallic Catalysts for Use in a Fuel Cell 査読有り

Matsumoto Takahiro, Kim Kyoungmok, Nakai Hidetaka, Hibino Takashi, Ogo Seiji

CHEMCATCHEM 5 巻 ( 6 ) 頁： 1368 - 1373 2013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：ChemCatChem

We report the successful increase in performance of a fuel cell based on organometallic catalysis. An organometallic [NiIIRuIV] peroxo complex functions as cathode catalyst and was designed following mechanistic consideration of the cell. It was confirmed that the organometallic [NiIIRuIV] peroxo catalyst could function in the fuel cell with a 240% increase in power output over our previous systems. This organometallic catalyst can act in both solid and solution phases and allows observation of the mechanism, hence providing us further opportunity for future improvement. © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

DOI： 10.1002/cctc.201200595

Proton-Conductor-Supported Ultra-Low Loading Pt-Rh Three-Way Catalysts 査読有り

Dong Xue, Nishida Masakazu, Hibino Takashi

JOURNAL OF PHYSICAL CHEMISTRY C 117 巻 ( 4 ) 頁： 1827 - 1832 2013年1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 Physical Chemistry C

Reaction of propane + NO + oxygen over PtRh was investigated using proton-conductive Sn0.9In0.1P2O7 (SIPO), Sn0.95Al0.05P2O7 (SAPO), Sn0.9Mg0.1P2O7 (SMPO), and Fe 0.5Nb0.5P2O7 (FNPO) materials as catalyst supports. The proton conductor-supported Pt-Rh catalysts (0.01 wt % Pt content and 0.005 wt % Rh content) showed significantly different activities: temperatures at which propane oxidation achieved 50% conversion (T 50%) were 313, 330, 405, and 550 C for Pt-Rh/FNPO, Pt-Rh/SIPO, Pt-Rh/SAPO, and Pt-Rh/SMPO, respectively; T50% values for NO reduction were 330, 386, 465, and greater than 600 C for Pt-Rh/FNPO, Pt-Rh/SIPO, Pt-Rh/SAPO, and Pt-Rh/SMPO, respectively. A similar tendency was also seen for the dependence of catalytic activity on space velocity. Only small differences in BET surface area and particle size were observed among FNPO, SIPO, SAPO, and SMPO. In addition, the dispersion state of PtRh was similar among the impregnated catalysts. Conversely, proton conductivity of these catalyst supports decreased in the order FNPO > SIPO > SAPO > SMPO. In particular, protons were most strictly restricted to the lattice oxide ions in SMPO. On the basis of these results, the catalytic activity of Pt-Rh/proton conductors was correlated with proton conduction in the bulk of the catalyst supports. © 2013 American Chemical Society.

DOI： 10.1021/jp312213x

An intermediate-temperature alkaline fuel cell using an Sn0.92Sb0.08P2O7-based hydroxide-ion-conducting electrolyte and electrodes 査読有り

Hibino Takashi, Kobayashi Kazuyo

JOURNAL OF MATERIALS CHEMISTRY A 1 巻 ( 4 ) 頁： 1134 - 1140 2013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 A

Although various types of anion exchange membrane fuel cells have been developed, few alkaline fuel cells capable of operating at temperatures above 100 °C have been reported, due to low chemical and thermal stability of the polymer electrolytes. Sn0.92Sb0.08P2O 7 is a hydroxide ion conductor that exhibits high conductivities ranging from 10-2 to 10-1 S cm-1 at elevated temperatures. This report describes the development of an intermediate- temperature alkaline fuel cell using an Sn0.92Sb0.08P 2O7-based electrolyte and electrodes. First, a dense and flexible composite membrane, composed of Sn0.92Sb 0.08P2O7 and polytetrafluoroethylene (PTFE), was synthesized and characterized. In the composite membrane, a homogeneous distribution of Sn0.92Sb0.08P2O7 particles was obtained at a thickness of 110 μm, yielding hydroxide ion conductivity of ∼10-2 S cm-1 in the temperature range between 75 and 200 °C. Next, the microstructure of the three-phase boundary in the electrode was established by incorporating Sn0.92Sb 0.08P2O7 particles into the electrode. Consequently, polarization resistance was reduced dramatically compared to that of the unmodified electrode. Finally, fuel cell tests were conducted using the optimized electrolyte and electrode. The peak power density was 76 mW cm -2 at 75 °C, 94 mW cm-2 at 100 °C, 114 mW cm -2 at 125 °C, 130 mW cm-2 at 150 °C, 132 mW cm-2 at 175 °C, and 147 mW cm-2 at 200 °C. High durability of the present fuel cell was also confirmed at 200 °C. © The Royal Society of Chemistry 2013.

DOI： 10.1039/c2ta00368f

Hydroxide ion conduction in molybdenum(VI)-doped tin pyrophosphate at intermediate temperatures 査読有り

Hibino Takashi, Kobayashi Kazuyo

JOURNAL OF MATERIALS CHEMISTRY A 1 巻 ( 23 ) 頁： 6934 - 6941 2013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 A

Research efforts focused on alkaline fuel cells have increased with the goal of commercialization. Anion exchange polymers are widely viewed as promising candidates for electrolyte membranes; however, the operating temperature of these polymers is limited to 80°C or lower. Operation of a fuel cell at elevated temperatures provides the anode catalyst with a high tolerance towards CO and enhances the electrode reaction kinetics. We present a new type of inorganic hydroxide ion-conducting compound that has the potential to meet the demands for intermediate temperature applications. A series of Sn1-xAxP2O7 (AVI = Mo and W) compounds were synthesized, of which Sn0.85Mo 0.15P2O7 exhibited the highest electrical conductivity over a wide temperature range (0.02 S cm-1@50°C, 0.07 S cm-1@100°C, 0.10 S cm-1@150°C, and 0.123 S cm-1@200 and 250°C). Such a high conductivity was also confirmed under conditions of fuel cell operation. The anion exchange capability of this compound was evaluated using spectroscopic and electrochemical analyses, the results of which indicated that hydroxide ions are incorporated into the compound by charge compensation for high valency cations and hydroxide ion conduction is predominant in the temperature range of 50-250°C. © 2013 The Royal Society of Chemistry.

DOI： 10.1039/c3ta10769h

Intermediate-temperature alkaline fuel cells with non-platinum electrodes 査読有り

Hibino Takashi, Kobayashi Kazuyo

JOURNAL OF MATERIALS CHEMISTRY A 1 巻 ( 24 ) 頁： 7019 - 7022 2013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 A

This report describes experimental results that demonstrate that less expensive Ru and Pd catalysts possess activity comparable to Pt when functioning as anode and cathode catalysts, respectively, at 200 °C, which is achieved by using a hydroxide-ion conductive Sn<inf>0.92</inf>Sb<inf>0.08</inf>P <inf>2</inf>O<inf>7</inf> electrolyte membrane. The resultant H<inf>2</inf>/air fuel cell yielded increasing peak power densities with temperature: 60 mW cm<sup>-2</sup> at 100 °C, 101 mW cm<sup>-2</sup> at 150 °C, and 152 mW cm<sup>-2</sup> at 200 °C. Note that the peak power density obtained for the Pt/C anode and cathode was 147 mW cm<sup>-2</sup> at 200 °C. High durability of the present fuel cell was also confirmed at 200 °C. © The Royal Society of Chemistry 2013.

DOI： 10.1039/c3ta11118k

Design of proton-conducting Sn(0.9)5Al(0.05)P(2)O(7) with a mesoporous structure 査読有り

Hibino Takashi, Kabayashi Kazuyo, Fujita Satoru

JOURNAL OF MATERIALS CHEMISTRY A 1 巻 ( 42 ) 頁： 13082 - 13088 2013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 A

Mesopores in inorganic materials are attractive and important spaces for the development of proton conductors, because capillary condensation of water molecules occurs at relatively low relative humidity (RH), allowing for fast transport of protons without excessive humidification. Most such mesoporous inorganic compounds are constructed of silica and titania. In this study, we adopt SnP2O7 and Sn0.95Al0.05P 2O7 as mesoporous frameworks. Since these pyrophosphates in themselves are proton-conducting materials, there may be synergy between the framework and mesopore spaces. Mesoporous SnP2O7 or Sn0.95Al0.05P2O7 was synthesized through a reaction between mesoporous SnO2 or Sn 0.95Al0.05O1.975 and phosphoric acid, respectively. At a reaction temperature of 250 °C, only the crystalline phase attributable to SnP2O7 was detected by X-ray diffraction. The obtained compounds showed hysteresis loops in the nitrogen gas adsorption/desorption isotherms, the analyses of which indicated mean pore diameters of ca. 7 nm for SnP2O7 and ca. 4 nm for Sn 0.95Al0.05P2O7. Partially destroyed hexagonal mesopores were observed in transmission electron spectroscopy observations of these compounds. The proton conductivity of the mesoporous SnP2O7 was more than one order of magnitude higher than that of the nonporous SnP2O7 in the temperature range of 50-200 °C. Furthermore, the dependence of the proton conductivity on the RH was much larger for the mesoporous SnP2O7 than for the nonporous SnP2O7. Temperature-programmed desorption analysis of water vapor revealed that water molecules filling the mesopores through capillary condensation are responsible for the high proton conductivity of the mesoporous SnP2O7 at low RH. More importantly, this capillary condensation effect was enhanced by doping SnP2O 7 with Al, which shifted the RH where the proton conductivity sharply increased to a lower value. The resultant proton conductivity at 150 °C reached 0.07 S cm-1 at only 14% RH. © 2013 The Royal Society of Chemistry.

DOI： 10.1039/c3ta12525d

An all-solid-state rechargeable aluminum-air battery with a hydroxide ion-conducting Sb(V)-doped SnP2O7 electrolyte 査読有り

Hibino Takashi, Kobayashi Kazuyo, Nagao Masahiro

JOURNAL OF MATERIALS CHEMISTRY A 1 巻 ( 47 ) 頁： 14844 - 14848 2013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 A

An anhydrous hydroxide ion conductor, Sn0.92Sb 0.08P2O7, can function as an electrolyte for aluminum-air batteries, where aluminum is oxidized to an aluminate species during discharge, and the aluminate species is reduced to aluminum by charging the cell. This battery generated an open-circuit voltage of ca. 1.6 V with a discharge capacity of ca. 800 mA h g-1electrode. © 2013 The Royal Society of Chemistry.

DOI： 10.1039/c3ta12707a

Room-temperature proton transport and its effect on thermopower in a solid ionic semiconductor, TTFCOONH4 査読有り

Kobayashi Yuka, Fujii Takenori, Terasaki Ichiro, Kino Hiori, Jin Yongcheng, Hibino Takashi, Kobayashi Tetsuya, Nishibori Eiji, Sawa Hiroshi, Yoshikawa Hideki, Terauchi Takeshi, Sumi Satoshi

JOURNAL OF MATERIALS CHEMISTRY A 1 巻 ( 16 ) 頁： 5089 - 5096 2013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 A

Ammonium proton in a solid ionic semiconductor, TTFCOONH4, is shown to be mobile under anhydrous conditions at room temperature by the hydrogen concentration cell method. Isotope substituted TTFCOOND4 exhibits a 2.2 H/D isotope effect in ion carrier mobility with TTFCOONH 4. First-principles calculations reveal that an efficient proton-transfer pathway via low-barrier N⋯H+⋯N hydrogen bonds reduces the activation energy to 0.12 eV, which is quite small and comparable to that reported in a bulk water system. The ac conductivity of TTFCOONH4 and TTFCOOND4 is similar at room temperature, reflecting similar hole carrier concentrations. In sharp contrast, the thermopower exhibits a large isotope effect: TTFCOONH4 shows 260 μV K-1, which is twice as large as that predicted by the hole carrier concentration and the value of TTFCOOND4, with 138 μV K-1. The 1.9 H/D isotope effect in thermopower closely relates to the 2.2 H/D isotope effect in ion carrier mobility. Proton carriers in the temperature gradient enhance thermopower without cancelling out the effect of holes in the solid state owing to possession of the same positive charge. © The Royal Society of Chemistry 2013.

DOI： 10.1039/c3ta00011g

Intermediate-temperature, non-humidified proton exchange membrane fuel cell with a highly proton-conducting Fe0.4Ta0.5P2O7 electrolyte 査読有り

Shen Yanbai, Heo Pilwon, Pak Chanho, Chang Hyuk, Hibino Takashi

ELECTROCHEMISTRY COMMUNICATIONS 24 巻 ( 1 ) 頁： 82 - 84 2012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：Electrochemistry Communications

Proton exchange membrane fuel cell (PEMFC) operation below 100 °C causes CO poisoning of the anode catalyst and results in low reaction kinetics of the cathode catalyst. In addition, operation at high relative humidity requires a large-sized humidifier, thereby increasing the complexity of the fuel cell system. These problems can be avoided by operating fuel cells above 100 °C and under low relative humidity. We report the performance of a non-humidified hydrogen-air PEMFC using Fe 0.4Ta 0.5P 2O 7 as an electrolyte in the temperature range of 100-225 °C. The PEMFC with this electrolyte achieves open-circuit voltages of 1000 mV or higher at all temperatures tested and demonstrates decreasing voltage drop with increasing temperature. The resultant fuel cell provides a peak power density of 341 mW cm - 2 at 225 °C, exhibiting stable chemical and thermal durability for 100 h. © 2012 Elsevier B.V.

DOI： 10.1016/j.elecom.2012.08.020

総説：中温プロトン伝導体のエネルギー・環境技術への応用

日比野高士

化学工業 63 巻 ( 10 ) 頁： 8-16 2012年10月

A solid-state particulate matter sensor based on electrochemical oxidation of carbon by active oxygen 査読有り

Shen Y. B., Harada T., Teranishi S., Hibino T.

SENSORS AND ACTUATORS B-CHEMICAL 162 巻 ( 1 ) 頁： 159 - 165 2012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：Sensors and Actuators, B: Chemical

The carbon oxidation activity and sensing performance of an electrochemical sensor incorporating a robust SnP 2O 7-SnO 2 composite ceramic as a solid electrolyte were investigated at an operating temperature of 200°C. Specific reactivity of the electrochemically formed active oxygen toward carbon was accomplished with a high current efficiency estimated from the four-electron reaction (C + 2H 2O → CO 2 + 4H + + 4e -). However, this reaction did not occur over the entire electrode layer, which resulted in low sensitivity and a slow response speed. This problem could be overcome by distributing a SnP 2O 7 ionomer over the working electrode at a level of several micrometers. Moreover, an additional benefit of the present sensor for practical applications is that little interference was encountered when sensing carbon at levels of 1000 ppm CO and 1000 ppm C 3H 8 in the sample gas. The resulting amperometric mode sensor could successfully produce a current signal that corresponded to the quantity of particulate matter (PM) in the bench test apparatus. These results demonstrate that the present sensor is able to continuously monitor the PM concentration while self-regenerating. © 2011 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.snb.2011.12.057

Alternating-Current Electrolysis for the Production of Phenol from Benzene 査読有り

Lee Byungik, Naito Hiroto, Nagao Masahiro, Hibino Takashi

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 51 巻 ( 28 ) 頁： 6961 - 6965 2012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：Angewandte Chemie - International Edition

Works both ways: Phenol was produced by both anodic and cathodic benzene oxidations over the V xO y-Sn 0.9In 0.1P 2O 7 electrode in an electrochemical cell, thus allowing the use of AC electrolysis for phenol production. AC electrolysis was found to be more efficient and selective toward phenol production than DC electrolysis. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

DOI： 10.1002/anie.201202159

Proton conduction in A(0.5)(III)B(0.5)(V)P(2)O(7) compounds at intermediate temperatures 査読有り

Shen Yanbai, Kojima Keijiro, Nishida Masakazu, Heo Pilwon, Choi Kyoung Hwan, Chang Hyuk, Hibino Takashi

JOURNAL OF MATERIALS CHEMISTRY 22 巻 ( 30 ) 頁： 14907 - 14915 2012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

Proton conductors capable of operation between 100 and 400 °C are attractive electrochemical materials due to their high utility value in energy and environmental applications. However, such proton conductors have not yet made headway in the marketplace, due to insufficient proton conductivity. Here, we present new types of metal pyrophosphates as promising candidates for intermediate temperature proton conductors. A series of AIII0.5BV0.5P2O7 (A IIIBV = InSb, SbSb, FeSb, GaNb, FeNb, YNb, GaTa, AlTa, FeTa, YTa, BiTa, and SmTa) compounds were synthesized, of which In 0.5Sb0.5P2O7, Fe 0.5Nb0.5P2O7, and Fe 0.5Ta0.5P2O7 exhibited the highest proton conductivities in the temperature ranges of 50-100 °C (0.045 S cm-1@100 °C), 100-200 °C (0.12 S cm-1@150 °C), and 200-400 °C (0.18 S cm-1@250 °C), respectively, in unhumidified air. The proton conductivity of these three compounds was further enhanced by the introduction of AIII or BV deficiency into the bulk. Consequently, Fe0.4Ta0.5P2O 7 exhibited the highest proton conductivity of 0.27 S cm-1 at 300 °C in unhumidified air. Such high proton conductivity values were also observed under fuel cell operating conditions. The environments of protons in the bulk of these compounds were monitored using Fourier transform infrared (FT-IR) spectroscopy, temperature-programmed desorption (TPD), and proton magic angle spinning (MAS) nuclear magnetic resonance (NMR) spectroscopy. Protons were incorporated into the compounds for charge-compensation of the deficient A III or BV cations, which results in an increase in the quantity of protons. More importantly, the mobility of the protons was also enhanced. Various electrochemical measurements demonstrate that proton conduction is dominant in these compounds, where the protons migrate according to a hopping mechanism. © The Royal Society of Chemistry 2012.

DOI： 10.1039/c2jm31887c

Hydroxide Ion Conducting Antimony(V)-Doped Tin Pyrophosphate Electrolyte for Intermediate-Temperature Alkaline Fuel Cells 査読有り

Hibino Takashi, Shen Yanbai, Nishida Masakazu, Nagao Masahiro

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 51 巻 ( 43 ) 頁： 10786 - 10790 2012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：Angewandte Chemie - International Edition

Ion conductor: A series of Sn 1-xA xP 2O 7 (A V=V, Nb, Ta, and Sb) compounds was synthesized, among which Sn 0.92Sb 0.08P 2O 7 (see picture) showed the highest hydroxide ion conductivity in the temperature range of 50-200 °C (0.08 S cm -1 at 100 °C and 0.05 S cm -1 at 200 °C). This high conductivity was also confirmed under fuel-cell-operating conditions. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

DOI： 10.1002/anie.201205022

Electrochemical Oxidation of Benzene to Phenol 査読有り

Lee Byungik, Naito Hiroto, Hibino Takashi

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 51 巻 ( 2 ) 頁： 440 - 444 2012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：Angewandte Chemie - International Edition

Gas-phase electrochemistry: The direct hydroxylation of benzene to phenol was investigated using an electrochemical cell. The production of phenol over a VO x anode was found to be significant at 50 °C. The resultant current efficiency for phenol production and selectivity toward phenol reached 76.5 and 94.7 %, respectively. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

DOI： 10.1002/anie.201105229

Proton conduction in non-doped and acceptor-doped metal pyrophosphate (MP2O7) composite ceramics at intermediate temperatures 査読有り

Sato Yousuke, Shen Yanbai, Nishida Masakazu, Kanematsu Wataru, Hibino Takashi

JOURNAL OF MATERIALS CHEMISTRY 22 巻 ( 9 ) 頁： 3973 - 3981 2012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

Proton conductors capable of operating in the temperature range of 100-600°C have received great interest for many application areas such as fuel cells, sensors, and electrolyzers; however, very few materials that can satisfy these demands have been reported to date. Here, we report a promising candidate for a solid electrolyte in intermediate-temperature electrochemical devices. First, MP 2O 7-MO 2 composite ceramics (M = Sn, Si, Ti, and Zr) were prepared by reacting a porous MO 2 substrate with an 85% H 3PO 4 solution at 600°C. Although all the tested MO 2 could react with H 3PO 4 to form the corresponding metal pyrophosphate layers on the surfaces of the exterior and interior substrate, the extent of MP 2O 7 growth in the obtained samples and their relative density were strongly dependent on the M species. These factors were the best for the SnP 2O 7-SnO 2 composite ceramic, yielding the highest electrical conductivity in the temperature range of interest. Next, different low valence cations (cation = Mg 2+, Sc 3+, Ga 3+, Y 3+, In 3+, La 3+, Sm 3+, Eu 3+, and Gd 3+) were doped into the SnP 2O 7-SnO 2 composite ceramic. The most positive effect on the electrical conductivity was observed when Sm 3+ was used as the dopant; the electrical conductivity of this sample was approximately one order of magnitude higher than that of the non-doped sample, especially at low temperatures below 250°C. Fourier transform infrared (FTIR) and proton magic angle spinning (MAS) nuclear magnetic resonance (NMR) analyses revealed that the quantity of protons incorporated in the SnP 2O 7 layer and their mobility were increased by the doping of Sm into the composite ceramic. As a consequence, the electrical conductivity of the Sm-doped SnP 2O 7-SnO 2 composite ceramic reached ∼10 -2 S cm -1 in the temperature range of 100-600°C. Proton conduction in this sample was also investigated by various electrochemical techniques. The protons function as the predominant charge carrier in the sample, and the proton transport number was almost unity in both static and dynamic conditions. © 2012 The Royal Society of Chemistry.

DOI： 10.1039/c2jm15335a

総説：ナノ局所電池デバイスのエネルギー・環境技術への応用

日比野高士

ケミカルエンジニヤリング 56 巻 ( 10 ) 頁： 48-54 2011年10月

Intermediate-temperature proton conductors and their applications to energy and environmental devices 査読有り

Hibino Takashi

JOURNAL OF THE CERAMIC SOCIETY OF JAPAN 119 巻 ( 1393 ) 頁： 677 - 686 2011年9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 the Ceramic Society of Japan

The development of proton conductors has proceeded rapidly in recent years. A number of organic or inorganic materials show proton conductivities of ∼10-2Scm-1 at temperatures below 100°C. However, although there is great current demand for proton conductors capable of operating in the temperature range of 100400° C in practical applications, very few materials that can satisfy this demand have been reported to date. Acceptor-doped SnP2O7 are promising candidate materials because their proton conductivities reach >10-1Scm-1 in the temperature range of interest. This paper presents an overview of the current status of acceptor-doped SnP2O7, highlighting the mechanism and kinetics of proton conduction and the development of electrochemical devices using these materials. New insights for proton insertion and conduction are proposed that use electrochemical techniques. Two approaches to designing SnP2O7-based composite electrolytes with good mechanical properties have also been developed for different operating temperatures. In addition, the benefits of intermediate-temperature operation using these materials are discussed in terms of practical applications, especially in fuel cells, exhaust sensors, and solid catalysts. © 2011 The Ceramic Society of Japan. All rights reserved.

DOI： 10.2109/jcersj2.119.677

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