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Study on the photoelectrochemical process for the conversion of small molecules in the gas phase by controlling the active species

Research Project

Project/Area Number 20H02525
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Review Section Basic Section 27030:Catalyst and resource chemical process-related
Research InstitutionTokyo Metropolitan University (2022-2023)
The University of Kitakyushu (2020-2021)

Principal Investigator

Amano Fumiaki  東京都立大学, 都市環境科学研究科, 教授 (10431347)

Project Period (FY) 2020-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥18,200,000 (Direct Cost: ¥14,000,000、Indirect Cost: ¥4,200,000)
Fiscal Year 2023: ¥2,600,000 (Direct Cost: ¥2,000,000、Indirect Cost: ¥600,000)
Fiscal Year 2022: ¥2,600,000 (Direct Cost: ¥2,000,000、Indirect Cost: ¥600,000)
Fiscal Year 2021: ¥2,600,000 (Direct Cost: ¥2,000,000、Indirect Cost: ¥600,000)
Fiscal Year 2020: ¥10,400,000 (Direct Cost: ¥8,000,000、Indirect Cost: ¥2,400,000)
Keywords光電気化学 / 半導体電極 / 光触媒 / 水分解 / メタン変換 / 水素製造 / メタン / 気相反応
Outline of Research at the Start

再生可能エネルギーの有効利用のためには、水蒸気や二酸化炭素のような気相中の小分子を燃料に転換するPower to Fuel技術の開発が必要とされている。特に、光や電気を使った常温反応プロセスの開発が期待されている。本研究では、独自に開発した全固体型の光電気化学システムを用いて、水蒸気やメタンの光電解反応について研究を進める。分子レベルでの活性種や反応機構の理解をもとに、気相小分子転換のための光電気化学反応プロセスの基盤技術を創出する。

Outline of Final Research Achievements

We investigated methane conversion reactions using a photoelectrochemical cell with a gas-diffusion tungsten trioxide (WO3) photoanode and a proton exchange membrane as a solid polymer electrolyte. When irradiated with blue light (with a wavelength of approximately 453 nm) in the presence of a humidified methane stream, ethane was produced with selectivity exceeding 60%, and the production rate increased with increasing incident light intensity. In contrast, under UV light irradiation, carbon dioxide production was dominant, and the selectivity for ethane production was reduced to be 30%. Electrolyte flow-type electron spin resonance measurements were performed to determine the Faradaic efficiency (current efficiency) of hydroxyl radical based on the photocurrent density value, and it was found that hydroxyl radicals as an active species are generated more efficiently under visible light irradiation compared to ultraviolet light irradiation.

Academic Significance and Societal Importance of the Research Achievements

再生可能エネルギーの有効活用を目的とし、光や電気を使って気相中の小分子を燃料に転換するPower to Fuel技術が注目されている。光電気化学反応は、液相中での物質転換反応には有効であるが、気相中の小分子の転換への応用は難しかった。本研究では、三相界面を適切に設計した全固体型の光電気化学システムの開発によって気相反応の評価を可能とし、水蒸気やメタンの光電解反応プロセスについて研究開発を行った。半導体電極や反応条件の検討によって、メタン分子を室温で活性化するための活性種が明らかとなり、光電解システムの耐久性を向上させるための学術的知見を得ることができた。

Report

(5 results)
  • 2023 Annual Research Report   Final Research Report ( PDF )
  • 2022 Annual Research Report
  • 2021 Annual Research Report
  • 2020 Annual Research Report
  • Research Products

    (40 results)

All 2024 2023 2022 2021 2020 Other

All Journal Article (23 results) (of which Int'l Joint Research: 1 results,  Peer Reviewed: 23 results,  Open Access: 6 results) Presentation (14 results) (of which Int'l Joint Research: 6 results,  Invited: 9 results) Book (1 results) Remarks (2 results)

  • [Journal Article] Methane Activation through Single-Electron Transfer from Water Molecules to the Surface States of Semiconductor Photocatalysts2024

    • Author(s)
      Amano Fumiaki、Beppu Kosuke、Sakata Yoshihisa
    • Journal Title

      ACS Catalysis

      Volume: 14 Issue: 10 Pages: 7788-7794

    • DOI

      10.1021/acscatal.4c00984

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Photoelectrochemical Conversion of Methane to Ethane and Hydrogen under Visible Light Using Functionalized Tungsten Trioxide Photoanodes with Proton Exchange Membrane2024

    • Author(s)
      Amano Fumiaki、Suzuki Souta、Tsushiro Keisuke、Ito Junji、Naito Tetsuro、Kubota Hiroshi
    • Journal Title

      ACS Applied Materials & Interfaces

      Volume: 16 Issue: 19 Pages: 24631-24640

    • DOI

      10.1021/acsami.4c02713

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Gas-fed photoelectrochemical reactions sustained by phosphotungstic acid as an inorganic surface electrolyte2024

    • Author(s)
      Amano Fumiaki、Tsushiro Keisuke、Akamoto Chiho
    • Journal Title

      Energy Advances

      Volume: 3 Issue: 3 Pages: 558-563

    • DOI

      10.1039/d3ya00568b

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Trapping of Intermediates of a Photocatalytic Oxygen Evolution Reaction in Overall Water Splitting2024

    • Author(s)
      Satoshi Nakayama Fumiaki Amano*, Souta Suzuki, Akira Yamakata, Kosuke Beppu
    • Journal Title

      ACS Applied Energy Materials

      Volume: 7 Issue: 4 Pages: 1398-1402

    • DOI

      10.1021/acsaem.3c03172

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Pd3Bi intermetallic particles prepared by the photodeposition method for photocatalytic ethane production from methane2024

    • Author(s)
      Singh Surya Pratap、Beppu Kosuke、Amano Fumiaki
    • Journal Title

      Chemical Communications

      Volume: 60 Issue: 19 Pages: 2673-2676

    • DOI

      10.1039/d3cc06121c

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Porous Transport Photoelectrodes Fabricated on Felt Substrates and Applications to Polymer Electrolyte Photoelectrochemistry2024

    • Author(s)
      Amano Fumiaki、Surya Rizki Marcony、Singh Surya Pratap
    • Journal Title

      ChemElectroChem

      Volume: 11 Issue: 8

    • DOI

      10.1002/celc.202300646

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Proton exchange membrane photoelectrochemical cell for water splitting under vapor feeding2024

    • Author(s)
      Amano Fumiaki、Tsushiro Keisuke
    • Journal Title

      Energy Materials

      Volume: 4 Issue: 1 Pages: 400006-400006

    • DOI

      10.20517/energymater.2023.77

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Facilitating methane conversion and hydrogen evolution on platinized gallium oxide photocatalyst through liquid-like water nanofilm formation2024

    • Author(s)
      Amano Fumiaki、Ishikawa Atsushi、Sato Hiromasa、Akamoto Chiho、Singh Surya Pratap、Yamazoe Seiji、Sugimoto Toshiki
    • Journal Title

      Catalysis Today

      Volume: 426 Pages: 114375-114375

    • DOI

      10.1016/j.cattod.2023.114375

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Photoelectrochemical C-H activation of methane to methyl radical at room temperature2023

    • Author(s)
      Amano Fumiaki、Shintani Ayami、Sakakura Tatsuya、Takatsuji Yoshiyuki、Haruyama Tetsuya
    • Journal Title

      Catalysis Science & Technology

      Volume: 13 Issue: 16 Pages: 4640-4645

    • DOI

      10.1039/d3cy00632h

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Ti-doped Fe2O3 Photoanodes on Three-Dimensional Titanium Microfiber Felt Substrate for Photoelectrochemical Oxygen Evolution Reaction2023

    • Author(s)
      Apriandanu Dewangga Oky Bagus、Nakayama Satoshi、Shibata Kento、Amano Fumiaki
    • Journal Title

      Electrochimica Acta

      Volume: 456 Pages: 142434-142434

    • DOI

      10.1016/j.electacta.2023.142434

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Clarification of Photoelectrochemical Oxygen Evolution Sites in TiO<sub>2</sub> Nanotube Array Electrodes by PbO<sub>2</sub> Deposition Method2023

    • Author(s)
      Amano Fumiaki、Nomura Shimpei、Tateishi Chihiro、Nakayama Satoshi
    • Journal Title

      Journal of The Electrochemical Society

      Volume: 170 Issue: 2 Pages: 026501-026501

    • DOI

      10.1149/1945-7111/acb4be

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Effect of two-step annealing on photoelectrochemical properties of hydrothermally prepared Ti-doped Fe2O3 films2023

    • Author(s)
      Apriandanu Dewangga Oky Bagus、Nomura Shinpei、Nakayama Satoshi、Tateishi Chihiro、Amano Fumiaki
    • Journal Title

      Catalysis Today

      Volume: 411-412 Pages: 113826-113826

    • DOI

      10.1016/j.cattod.2022.06.041

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Highly Active Rutile TiO2 for Photocatalysis under Violet Light Irradiation at 405 nm2022

    • Author(s)
      Amano Fumiaki、Yamamoto Akira、Kumagai Jun
    • Journal Title

      Catalysts

      Volume: 12 Issue: 10 Pages: 1079-1079

    • DOI

      10.3390/catal12101079

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Effects of Hydroxy Groups in Anthraquinone Dyes on Photocatalytic Activity of Visible-light-sensitized Pt-TiO2 for Hydrogen Evolution2022

    • Author(s)
      Amano Fumiaki、Akaki Yasukazu、Yamakata Akira
    • Journal Title

      Catalysis Surveys from Asia

      Volume: 27 Issue: 1 Pages: 75-83

    • DOI

      10.1007/s10563-022-09370-y

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Electrochemical impedance spectroscopy of WO3 photoanodes on different conductive substrates: The interfacial charge transport between semiconductor particles and Ti surface2022

    • Author(s)
      Amano Fumiaki、Koga Shinichiro
    • Journal Title

      Journal of Electroanalytical Chemistry

      Volume: 921 Pages: 116685-116685

    • DOI

      10.1016/j.jelechem.2022.116685

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Improvement of water splitting activity of silver-excess AgTaO3 photocatalysts via nitric acid washing treatment2022

    • Author(s)
      Amano Fumiaki、Nakayama Satoshi
    • Journal Title

      Journal of Environmental Chemical Engineering

      Volume: 10 Issue: 4 Pages: 108089-108089

    • DOI

      10.1016/j.jece.2022.108089

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Hydroxyl Radical Formation on Metal-Loaded Ga2O3 Photocatalysts for Dehydrogenative Coupling of Methane to Ethane with Water2022

    • Author(s)
      Amano Fumiaki、Ishimaru Mizuki
    • Journal Title

      Energy Fuels

      Volume: - Issue: 10 Pages: 5393-5402

    • DOI

      10.1021/acs.energyfuels.2c00401

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Structure-Stability Relationship of Amorphous IrO2-Ta2O5 Electrocatalysts on Ti Felt for Oxygen Evolution in Sulfuric Acid2022

    • Author(s)
      Amano Fumiaki、Furusho Yoshiyuki、Yamazoe Seiji、Yamamoto Muneaki
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 126 Issue: 4 Pages: 1817-1827

    • DOI

      10.1021/acs.jpcc.1c09775

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Direct Electrochemical Visualization of the Orthogonal Charge Separation in Anatase Nanotube Photoanodes for Water Splitting2022

    • Author(s)
      Makarova Marina V.、Amano Fumiaki、Nomura Shinpei、Tateishi Chihiro、Fukuma Takeshi、Takahashi Yasufumi、Korchev Yuri E.
    • Journal Title

      ACS Catalysis

      Volume: 12 Issue: 2 Pages: 1201-1208

    • DOI

      10.1021/acscatal.1c04910

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Effect of Adding Polyethylene Glycol to the Precursor Solution of Amorphous IrO<sub>2</sub>-Ta<sub>2</sub>O<sub>5</sub> Electrocatalysts for Oxygen Evolution Reaction2021

    • Author(s)
      FURUSHO Yoshiyuki、AMANO Fumiaki
    • Journal Title

      Electrochemistry

      Volume: 89 Issue: 3 Pages: 234-238

    • DOI

      10.5796/electrochemistry.21-00001

    • NAID

      130008034676

    • ISSN
      1344-3542, 2186-2451
    • Year and Date
      2021-05-05
    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Photoelectrochemical stability of WO3/Mo-doped BiVO4 heterojunctions on different conductive substrates in acidic and neutral media2021

    • Author(s)
      Ta Chau Xuan Minh、Furusho Yoshiyuki、Amano Fumiaki
    • Journal Title

      Applied Surface Science

      Volume: 548 Pages: 149251-149251

    • DOI

      10.1016/j.apsusc.2021.149251

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Methane coupling and hydrogen evolution induced by palladium-loaded gallium oxide photocatalysts in the presence of water vapor2021

    • Author(s)
      Ishimaru Mizuki、Amano Fumiaki、Akamoto Chiho、Yamazoe Seiji
    • Journal Title

      Journal of Catalysis

      Volume: - Pages: 192-200

    • DOI

      10.1016/j.jcat.2021.03.024

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] A Macroporous-Structured WO3/Mo-Doped BiVO4 Photoanode for Vapor-Fed Water Splitting under Visible Light Irradiation2020

    • Author(s)
      Ta Chau Xuan Minh、Akamoto Chiho、Furusho Yoshiyuki、Amano Fumiaki
    • Journal Title

      ACS Sustainable Chemistry & Engineering

      Volume: 8 Issue: 25 Pages: 9456-9463

    • DOI

      10.1021/acssuschemeng.0c02331

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Presentation] Activation of Methane Mediated by Water Molecules on the Surface of Semiconductor Photocatalysts2023

    • Author(s)
      F. Amano, S. Nakayama, and K. Beppu
    • Organizer
      The 19th Korea-Japan Symposium on Catalysis, Seoul, Korea
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Proton Exchange Membrane Photoelectrochemical Cell and Gas-Diffusion Photoanodes for Vapor-Fed Water Splitting2023

    • Author(s)
      F. Amano
    • Organizer
      The Annual Nanotechnology Conference 2023, Warsaw, Poland
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Photocatalytic Dehydrogenative Coupling of Methane in the Presence of Water Vapor2022

    • Author(s)
      Fumiaki Amano
    • Organizer
      Post Symposium of TOCAT9, 60th Aurora seminar, The 9th International Symposium of Institute for Catalysis
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 気相中の小分子変換を志向した光電気化学系の開発2022

    • Author(s)
      天野史章
    • Organizer
      触媒学会(西日本支部)第60回触媒研究懇談会
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] 光電気化学触媒とメタン転化2022

    • Author(s)
      天野史章
    • Organizer
      2022年度高難度選択酸化反応研究会シンポジウム
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] Vapor-Fed Photoelectrochemical Water Splitting by Gas Diffusion Photoelectrodes2022

    • Author(s)
      Fumiaki Amano
    • Organizer
      The 9th Tokyo Conference on Advanced Catalytic Science and Technology (TOCAT9)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Gas-Phase Photoelectrochemical Reactions using WO3 Photoanode Decorated with Tungsto(VI) Phosphoric Acid2022

    • Author(s)
      Fumiaki Amano
    • Organizer
      The 73rd Annual Meeting of the International Society of Electrochemistry (ISE)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Fe2O3 Photoanodes on Different Conductive Substrates for Photoelectrochemical Oxygen Evolution Reaction2022

    • Author(s)
      Dewangga Oky Bagus Apriandanu, Shinpei Nomura, Satoshi Nakayama, Kento Shibata, Fumiaki Amano
    • Organizer
      The 73rd Annual Meeting of the ISE
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 半導体光触媒表面上での水分子を介したメタンの活性化2022

    • Author(s)
      天野史章・中山智志・別府孝介
    • Organizer
      第131回触媒討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] ガス拡散半導体電極の開発と光電気化学的な水蒸気分解による水素製造2022

    • Author(s)
      天野史章
    • Organizer
      日本化学会 第102春季年会 イノベーション共創プログラム(CIP)
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] 気相小分子の光電解反応2021

    • Author(s)
      天野史章
    • Organizer
      第437回触媒科学研究所コロキウム
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] 酸化物光触媒の設計と光電解プロセスへの応用2021

    • Author(s)
      天野史章
    • Organizer
      2020年度 第4回人工光合成研究拠点 講演会
    • Related Report
      2020 Annual Research Report
    • Invited
  • [Presentation] 光エネルギーを利用した気相小分子の転換反応2021

    • Author(s)
      天野史章
    • Organizer
      日本化学会 第101春季年会 (2021)
    • Related Report
      2020 Annual Research Report
    • Invited
  • [Presentation] 気相小分子を転換するための光電解反応プロセス2020

    • Author(s)
      天野史章
    • Organizer
      2020年 日本化学会九州支部 秋期研究発表会
    • Related Report
      2020 Annual Research Report
    • Invited
  • [Book] メタンと二酸化炭素~ その触媒的化学変換技術の現状と展望 ~第4章第2節「光駆動型メタンカップリング反応」2023

    • Author(s)
      天野史章
    • Total Pages
      9
    • Publisher
      シーエムシー・リサーチ
    • ISBN
      9784910581361
    • Related Report
      2022 Annual Research Report
  • [Remarks] ナノ構造光電極の電荷分離機構を実空間で可視化 ~太陽光水分解の材料開発を促進~

    • URL

      https://nanolsi.kanazawa-u.ac.jp/post-19160/

    • Related Report
      2021 Annual Research Report
  • [Remarks] ナノ構造光電極の電荷分離機構を実空間で可視化 ~太陽光水分解の材料開発を促進~

    • URL

      https://www.jst.go.jp/pr/announce/20220107-2/index.html

    • Related Report
      2021 Annual Research Report

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Published: 2020-04-28   Modified: 2025-01-30  

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