研究者詳細 - 日比野　高士

論文 - 日比野　高士

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Electrochemical production of methanol and hydrogen from biomass waste 査読有り

Zichun Xiong, Kazuyo Kobayashi, Aki Miyawaki, Shinya Teranishi, Takashi Hibino

Electrochemistry Communications 頁： 107862 2025年1月

Electro-oxidative extraction of methanol from lignin using a three-dimensional graphite anode 招待有り査読有り

Zichun Xiong, Kazuyo Kobayashi, Aki Miyawaki, Shinya Teranishi, Yoshiharu Sawada, Takashi Hibino

ChemElectroChem 頁： e202400464 2024年11月

総説：廃棄バイオマスの電解酸化によるエネルギー・資源変換招待有り

日比野高士

触媒 66 巻 ( 6 ) 2024年12月

総説：廃棄バイオマスを利用した燃料電池と電気分解招待有り

日比野高士

日本化学会「化学と教育」 72 巻 ( 6 ) 2024年6月

Electrochemical extraction of methanol from lignin under mild conditions 査読有り

Takashi Hibino, Kazuyo Kobayashi, Dongwen Zhou, Siyuan Chen, Anatoly Zinchenko, Shinya Teranishi, Aki Miyawaki, Yoshiharu Sawada

Applied Catalysis B: Environmental 341 巻頁： 123328 2023年9月

Alternating current electrolysis for individual synthesis of methanol and ethane from methane in a thermo-electrochemical cell 査読有り

Takashi Hibino, Kazuyo Kobayashi, Masahiro Nagao, Dongwen Zhou, Siyuan Chen, Yuta Yamamoto

ACS Catalysis 13 巻頁： 8890 - 8901 2023年6月

Two-stage electrolysis of H2O and CO2 to methanol: CO2-to-methane reduction at the cathode and subsequent methane-to-methanol oxidation at the anode 査読有り

Hibino Takashi, Kobayashi Kazuyo, Nagao Masahiro, Dongwen Zhou, Siyuan Chen

JOURNAL OF MATERIALS CHEMISTRY A 10 巻 ( 42 ) 頁： 22718 - 22729 2022年11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：Journal of Materials Chemistry A

Co-electrolysis of H2O and N/C sources to valuable chemicals has the potential to contribute to global warming mitigation. We here report the electrochemical conversion of H2O and CO2 into methanol in a gas flow system at temperatures between 100 and 200 °C. CO2 was reduced to methane with voltage-boosted H2 at a Ru/C cathode. Introduced Fe2O3 nanoparticles promoted the adsorption and activation of CO2 on the surface of Ru because of their high redox activity. Methane was oxidized to methanol through the formation of ˙CH3 and active oxygen species at a Pt anode. The addition of Au to the anode enhanced the selectivity toward methanol by reducing the activity of Pt in the complete oxidation of methanol. Combining these processes with gas penetration into the electrolyte membrane enabled the synthesis of methanol from H2O and CO2, with a maximum faradaic efficiency of 54%. This work establishes a methodology for providing a good balance between the activity and selectivity of electrodes for the CO2 reduction reaction.

DOI： 10.1039/d2ta04011e

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Solid oxide fuel cell using plastic waste directly as fuel 査読有り

Hibino Takashi, Kobayashi Kazuyo, Hitomi Takuma

CHEMISTRY LETTERS 50 巻 ( 10 ) 頁： 1729 - 1732 2021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：Chemistry Letters

Direct utilization of combustible waste as an energy resource is very attractive for improving waste-to-energy conversion efficiency. Herein, we report a high-performance solid oxide fuel cell (SOFC) that can be supplied continuously with plastic waste as a fuel. Iron(III) oxide powder functioned as a pseudofuel in the ion transfer process and as a catalyst for gasification of the plastic. The resultant SOFC provided peak power densities of 0.71, 0.68, and 0.57 W cm12 for nylon 66, polyethylene, and polystyrene, respectively.

DOI： 10.1246/cl.210321

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Biomass solid oxide fuel cell using solid weed waste as fuel 査読有り

Hibino Takashi, Kobayashi Kazuyo, Hitomi Takuma

ELECTROCHIMICA ACTA 388 巻頁： 138681 2021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：Electrochimica Acta

Weed waste is an abundant and carbon-neutral feedstock for energy recovery. A potential approach to improve the efficiency of waste-to-energy conversion is the application of a fuel-cell-type reactor to the treatment system to generate electricity from the feedstock, with high power and energy density. Herein, we report a solid oxide fuel cell (SOFC) that directly uses solid weed waste as fuel. Grasses tested in this study were Miscanthus sinensis, Solidago canadensis, and Pueraria montana. The conversion reactions for these grasses, especially in situ gasification, were effectively catalyzed at 800 °C by a thin layer of a silver–iron(III) oxide mixture that was deposited onto the anode substrate. The use of Solidago canadensis and Pueraria montana provided the highest power density (0.41 W cm−2) and energy density (0.42 Wh g−1), respectively, which were closely related to their lignin and ash contents. Importantly, this SOFC exhibited good performance not only in batch mode but also in continuous free-fall mode.

DOI： 10.1016/j.electacta.2021.138681

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Solid oxide fuel cell using municipal solid waste directly as fuel: biomass, resin, plastic, and food waste 査読有り

Hibino Takashi, Kobayashi Kazuyo, Teranishi Shinya, Hitomi Takuma

ACS SUSTAINABLE CHEMISTRY & ENGINEERING 9 巻 ( 8 ) 頁： 3124 - 3136 2021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：ACS Sustainable Chemistry and Engineering

Municipal solid waste has received significant attention in advanced waste treatment engineering. A recent trend emphasizing its significance is the utilization of waste as an energy source with high efficiency and low cost. This report describes a waste-to-energy fuel cell that uses biomass, resin, plastic, and food waste directly as fuels at a temperature of 800 °C. A Fe2O3 anode demonstrated the best catalytic effect for the anode reaction among various investigated transition-metal oxides. Fe2O3 was reduced to FeO by pyrolysis gases or solid fuel at the open-circuit voltage and was then gradually reoxidized to its initial oxidation state by anodic polarization. The gasification reaction of carbon with carbon dioxide, i.e., the Boudouard reaction, was substantially catalyzed during discharge of the cell. Cell performance was dependent on the quantity and type of solid fuel: polyethylene terephthalate provided the highest power density of 0.57 W cm-2, whereas lignin presented the highest energy density of 0.83 Wh g-1 (lignin). Two distinctive features of this fuel cell are that the organic components of the solid fuels are almost completely consumed by discharge of the cell and that solid fuels can be supplied in both batch and free-fall modes.

DOI： 10.1021/acssuschemeng.0c07657

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A NiRhS fuel cell catalyst - lessons from hydrogenase 査読有り

Ogo S., Ando T., Minh L.T.T., Mori Y., Matsumoto T., Yatabe T., Yoon K.S., Sato Y., Hibino T., Kaneko K.

Chemical Communications 56 巻 ( 79 ) 頁： 11787 - 11790 2020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：Chemical Communications

We present a novel fuel cell heterogeneous catalyst based on rhodium, nickel and sulfur with power densities 5-28% that of platinum. The NiRhS heterogeneous catalyst was developedviaa homogeneous model complex of the [NiFe]hydrogenases (H2ases) and can act as both the cathode and anode of a fuel cell.

DOI： 10.1039/d0cc04789a

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Ionic conductive and photocatalytic properties of cementitious materials: calcium silicate hydrate and calcium aluminoferrite 査読有り

Nagao Masahiro, Kobayashi Kazuyo, Jin Yongcheng, Maruyama Ippei, Hibino Takashi

JOURNAL OF MATERIALS CHEMISTRY A 8 巻 ( 30 ) 頁： 15157 - 15166 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：Journal of Materials Chemistry A

Few studies have reported the ionic conductive and photoactive properties of cementitious materials, owing to the compositional and structural variations of cement paste. The present report focuses on calcium silicate hydrate (C-S-H) and tetracalcium aluminoferrite (C4AF), prepared individually from pure constituent elements. C-S-H is an ionic conductor with a conductivity ranging from 10-4 to 10-3 S cm-1 in humidified air at temperatures between 60 and 100 °C. The hydroxide ions present in the mesopores of C-S-H as basic O-H groups were determined to be the major charge carriers, and the faradaic efficiency for the water oxidation reaction was estimated to be approximately 100%. C4AF is a mixed ionic n-type electronic conductor, particularly at high oxygen partial pressures. The conductivity of this compound was several times lower than that of C-S-H under the same humidity and temperature conditions, not only because of the bulk resistance but also the grain boundary resistance. C4AF and the hydrates exhibited photovoltaic and photocatalytic responses for water splitting and methylene blue degradation, respectively. These results indicate the important contribution of C-S-H and hydrated C4AF to the electrochemical and photochemical properties of cement paste.

DOI： 10.1039/d0ta04866f

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Fuel cell and electrolyzer using plastic waste directly as fuel 査読有り

Hori Tetsuya, Kobayashi Kazuyo, Teranishi Shinya, Nagao Masahiro, Hibino Takashi

WASTE MANAGEMENT 102 巻頁： 30 - 39 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：Waste Management

The effective utilization of plastic waste, including its use as an energy or chemical resource, has attracted much attention. Nevertheless, energy recovery from plastics via incineration generates air pollutants and toxic compounds, while chemical conversion requires significant energy inputs, especially in the case of gasification. Herein, we report the electrochemical conversion of plastics into electricity or hydrogen without the use of special procedures. When a mixture of plastic solid combined with an acidic solution was fed into an electrochemical cell, the solid was found to dissolve in the solution at 100 °C or higher, followed by the release of protons from the anode to the cathode according to a multi-electron oxidation reaction. This oxidation reaction required an anode that was sufficiently porous so as to allow transport of the reactants. Taking the sponge sample as an example, the dissolved polyurethane had a molecular weight of 2000 or higher, the transport of which was facilitated using a carbon support with a pore diameter of approximately 10 nm. In addition, carbon black having an ordered porous structure exhibited better reagent transport compared to a disordered porous carbon black with similar pore diameters. As a consequence, this cell continuously provided power densities on the order of mW cm−2 in the fuel cell mode and generated hydrogen at a low cell voltage of 0.55 V in the electrolyzer mode, using plastics as fuels at an operational temperature of 200 °C.

DOI： 10.1016/j.wasman.2019.10.019

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A cellulose electrolysis cell with metal-free carbon electrodes 査読有り

Li Yaorong, Nagao Masahiro, Kobayashi Kazuyo, Jin Yongcheng, Hibino Takashi

CATALYSTS 10 巻 ( 1 ) 頁： 106 2020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：Catalysts

Biomass raw materials, including agricultural residues, collected weeds, and wood chips, are important feedstocks for hydrogen production. Numerous attempts have been made to electrolyze biomass directly or indirectly to hydrogen because these processes allow for the production of hydrogen with less power consumption than water electrolysis. However, expensive metal-based electrocatalysts are needed, especially for the cathode reaction, in the electrolysis cells. Results from the present study demonstrate the production of hydrogen directly from cellulose, using an optimal mesoporous carbon as the cathode in addition to a partially oxygenated carbon anode at a temperature of 150 °C, with an electrolysis onset voltage of ca. 0.2 V, a current density of 0.29 A cm–2 at an electrolysis voltage of 1 V, and a current efficiency of approximately 100% for hydrogen production. These characteristics were comparable to those recorded when using a Pt/C anode and cathode under the same conditions. The sp2 planes of the carbon allowed π electrons to be donated to protons at the cathode. In addition, the mesoporous structure provided a sufficient amount of sp2 planes on the surface of the cathode.

DOI： 10.3390/catal10010106

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Humidity Driven Transition from Insulator to Ionic Conductor in Portland Cement 査読有り

Nagao Masahiro, Kobayashi Kazuyo, Hori Tetsuya, Li Yaorong, Hibino Takashi

MATERIALS 12 巻 ( 22 ) 頁： 3701 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：Materials

This work aims to assess ionic conduction in anhydrous cement particles and hydrated cement pastes with aging periods of 5-25 days. When a cement sample was humidified (relative humidity = 100%) over the range of 50-100 0C, it exhibited bulk conductivities of 10-3-10-2 S cm-1, regardless of the hydration level, whereas the interfacial conductivities varied in the range of 10-7-10-3 S cm-1, depending on the structural defects or conduction pathways of the sample. Both the bulk and interfacial conductivities were increased to 0.01 S cm-1 or higher at 100 0C, although the sample required previous moistening with water mist. The major charge carrier in the sample was determined to be hydroxide ions, and the total ion transport number was approximately 1. Exposing the sample to a mixture of carbon dioxide and water vapor caused a decrease in the bulk and interfacial conductivities; however, the bulk conductivity was returned to the initial value by treatment with an acid.

DOI： 10.3390/ma12223701

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Electrolysis of humidified methane to hydrogen and carbon dioxide at low temperatures and voltages 査読有り

Hori Tetsuya, Ma Qiang, Kobayashi Kazuyo, Nagao Masahiro, Teranishi Shinya, Hibino Takashi

INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 44 巻 ( 5 ) 頁： 2454 - 2460 2019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：International Journal of Hydrogen Energy

Considerable amounts of hydrogen are produced from fossil fuels. In recent years, natural gas and biogas have received attention as important feedstocks for hydrogen production, because methane, their main component, is hydrogen rich and readily available. Methane steam reforming is the major industrial route for hydrogen production, but requires high temperature due to endothermic nature of the reaction. This report presents a new green technology for the efficient and ecological production of hydrogen from methane. A humidified methane was electrolyzed to hydrogen and carbon dioxide at low onset cell voltages (ca. 0.3–0.4 V), depending on the temperature (150–250 °C). Almost all currents were used for the production of hydrogen and carbon dioxide. Hydroxyl radicals generated from water vapor during the electrolysis played an important role as an active oxygen for the methane oxidation reaction at the anode. This is the first report on the production of hydrogen from methane at both low temperatures and voltages.

DOI： 10.1016/j.ijhydene.2018.12.044

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Intermediate-temperature electrolysis of energy grass Miscanthus sinensis for sustainable hydrogen production 査読有り

Ito Masaya, Hori Tetsuya, Teranishi Shinya, Nagao Masahiro, Hibino Takashi

SCIENTIFIC REPORTS 8 巻 ( 1 ) 頁： 16186 2018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：Scientific Reports

Biohydrogen produced from the electrolysis of biomass is promising because the onset voltages are less than 1.0 V and comparable to those of water and alcohol-water electrolysis. The present study focuses on Miscanthus sinensis as a model grass because of its abundance and ease of cultivation in Japan. The electrochemical performance and hydrogen formation properties of electrolysis cells using grass as a biohydrogen source were evaluated at intermediate temperature to achieve electrolysis. The components, such as holocellulose, cellulose, lignin, and extractives, were separated from Miscanthus sinensis to understand the reactions of Miscanthus sinensis in the electrolysis cell. The relatively high resistivity and low current-voltage performance of an electrolysis cell using lignin were responsible for degradation of the electrolysis properties compared to those with pure cellulose or holocellulose as biohydrogen resources. Biohydrogen was formed according to Faraday’s law and evolved continuously at 0.1 A cm−2 for 3,000 seconds.

DOI： 10.1038/s41598-018-34544-y

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Direct electrolysis of waste newspaper for sustainable hydrogen production: an oxygen-functionalized porous carbon anode 査読有り

Hibino Takashi, Kobayashi Kazuyo, Ito Masaya, Nagao Masahiro, Fukui Mai, Teranishi Shinya

APPLIED CATALYSIS B-ENVIRONMENTAL 231 巻頁： 191 - 199 2018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：Applied Catalysis B: Environmental

Biomass electrolysis enables hydrogen (H2) production at onset voltages of less than 1 V, depending on the fuel species. However, biofuel derived from biomass not categorized as food and produced from environmentally friendly processes is needed for the development of sustainable strategies. In addition, the biofuel should not require special and expensive procedures for processing. The present report describes the direct electrolysis of waste newspaper for H2 production. Cellulose and lignin included in the newspaper were subject to dissolution and hydrolysis in a phosphoric acid solvent at the anode in a temperature range of 100–175 °C. The resulting decomposition products were electrolyzed to H2 and carbon dioxide (CO2), at low onset voltages (ca. 0.2 V) and high current efficiencies (H2: 1.0, CO2: 0.9). Carbon black functionalized with carbonyl groups showed greater catalytic activity than a Pt/C catalyst for the anode reaction. H2 yield reached ca. 0.2 g per 1 g of newspaper in a batch cell. H2 was produced continuously in a current-density range of 0.15–0.25 A cm−2 while maintaining plateau-like voltage behavior in a flow cell. The energy consumed for electrolysis at a current density of 0.15 A cm−2 was as low as 1.27 kWh (Nm3)−1.

DOI： 10.1016/j.apcatb.2018.03.021

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Efficient Hydrogen Production by Direct Electrolysis of Waste Biomass at Intermediate Temperatures 査読有り

Hibino Takashi, Kobayashi Kazuyo, Ito Masaya, Ma Ojang, Nagao Masahiro, Fukui Mai, Teranishi Shinya

ACS SUSTAINABLE CHEMISTRY & ENGINEERING 6 巻 ( 7 ) 頁： 9360 - 9368 2018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：ACS Sustainable Chemistry and Engineering

Biomass has been considered as an alternative feedstock for energy and material supply. However, the lack of high-efficiency and low-cost processes for biomass utilization and conversion hinders its large-scale application. This report describes electrochemical hydrogen production from waste biomass that does not require large amounts of energy or high production costs. Hydrogen was produced by the electrolysis of bread residue, cypress sawdust, and rice chaff at an onset cell voltage of ca. 0.3 V, with high current efficiencies of approximately 100% for hydrogen production at the cathode and approximately 90% for carbon dioxide production at the anode. The hydrogen yields per 1 mg of the raw material were 0.1-0.2 mg for all tested fuels. Electrolysis proceeded continuously at plateau voltages that were proportional to the current. These characteristics were attributable to the high catalytic activity of the carbonyl-group functionalized mesoporous carbon for the anode reaction, and that the major components of biomass such as cellulose, starch, lignin, protein, and lipid were effectively utilized as fuels for hydrogen production.

DOI： 10.1021/acssuschemeng.8b01701

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Hydrogen Production by Direct Lignin Electrolysis at Intermediate Temperatures 査読有り

Hibino Takashi, Kobayashi Kazuyo, Nagao Masahiro, Teranishi Shinya

CHEMELECTROCHEM 4 巻 ( 12 ) 頁： 3032 - 3036 2017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：ChemElectroChem

Hydrogen is produced conventionally by electrolyzing water or water vapor at onset voltages greater than 1 V, providing motivation for the development of more efficient electrolysis processes for a hydrogen economy. Numerous attempts have been made to use ethanol as a fuel for hydrogen production because this process reduces the electrolysis onset voltage significantly. However, ethanol feedstock from lignocellulose requires greater amounts of energy and results in higher production costs compared to those using starch as the feedstock. The current study describes direct lignin electrolysis at an onset voltage of ca. 0.25 V, with high current efficiencies of approximately 100 % for hydrogen production at the cathode and approximately 85 % for carbon dioxide production at the anode. Addition of H3PO4-impregnated lignin to the anode of a PtFe/C|Sn0.9In0.1P2O7 (150 μm)|Pt/C cell enabled hydrogen production at a temperature of 150 °C.

DOI： 10.1002/celc.201700917

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