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光触媒活性サイトその場分析法開発に関する国際共同研究

Research Project

Project/Area Number 20KK0116
Research Category

Fund for the Promotion of Joint International Research (Fostering Joint International Research (B))

Allocation TypeMulti-year Fund
Review Section Medium-sized Section 28:Nano/micro science and related fields
Research InstitutionOsaka Metropolitan University (2022-2023)
Osaka City University (2020-2021)

Principal Investigator

吉田 朋子  大阪公立大学, 人工光合成研究センター, 教授 (90283415)

Co-Investigator(Kenkyū-buntansha) 東 正信  大阪公立大学, 人工光合成研究センター, 特任准教授 (10711799)
山本 旭  京都大学, 人間・環境学研究科, 助教 (30769443)
山本 宗昭  大阪公立大学, 人工光合成研究センター, 特任助教 (50823712)
Project Period (FY) 2020-10-27 – 2025-03-31
Project Status Granted (Fiscal Year 2023)
Budget Amount *help
¥18,590,000 (Direct Cost: ¥14,300,000、Indirect Cost: ¥4,290,000)
Fiscal Year 2024: ¥4,680,000 (Direct Cost: ¥3,600,000、Indirect Cost: ¥1,080,000)
Fiscal Year 2023: ¥4,030,000 (Direct Cost: ¥3,100,000、Indirect Cost: ¥930,000)
Fiscal Year 2022: ¥4,810,000 (Direct Cost: ¥3,700,000、Indirect Cost: ¥1,110,000)
Fiscal Year 2021: ¥2,990,000 (Direct Cost: ¥2,300,000、Indirect Cost: ¥690,000)
Fiscal Year 2020: ¥2,080,000 (Direct Cost: ¥1,600,000、Indirect Cost: ¥480,000)
KeywordsXAFS / EELS / 光触媒 / X線励起発光 / 定量的構造解析 / XAFS測定 / XANES解析法 / X線発光 / 放射光分光 / 電子分光
Outline of Research at the Start

本提案では,反応中に刻々と変化する固体光触媒活性サイトを抽出し,その場観察するための分析法を世界に先駆けて構築する.具体的には,触媒の局所構造・化学状態解析に有用なX線吸収分光法(XAFS)を活性サイト分析法に発展させるために,化学状態を選別した測定法や定量的解析法を共同開発する.この方法論を電子線エネルギー損失分光法(EELS)に応用し,固体光触媒の活性サイトの分布を定量的,且つ原子レベルで可視化する高空間分解分析法へと発展させる.本提案では,研究代表者を中心としてイタリア側研究拠点に出向き,国際共同研究を強力に推進すると共に,国際的に活躍する若手研究者を育成することも大きな目標としている.

Outline of Annual Research Achievements

透過型電子顕微鏡を用いて得られる電子エネルギー損失分光スペクトル(Electron Energy Loss Spectroscopy : EELS)の中のエネルギー損失吸収端微細構造(Energy Loss Near Edge Structure: ELNES)はXANESと同様の情報を与える.この特質に着目し,今年度はELNESを半導体光触媒(金属酸化物触媒)に添加した不純物元素の化学状態解析に応用した.Padova大学が得意とするイオン注入法を用いて,紫外光照射下でのみ触媒機能を発現する金属酸化物光触媒に対して,Nなどの各種アニオンを添加し可視光応答化(可視光照射下でも触媒機能を発現させること)を試みた.具体的には,添加したアニオン種を対象としたELNESスペクトルを測定することで,可視光応答化したアニオン種(活性種)と応答化しなかったアニオン種(不活性種)の化学状態をそれぞれ同定することに成功した.更にXANESスペクトルを利用した定量的化学状態解析法をELNESスペクトルにも応用することで,活性種と不活性種に由来するELNESスペクトルを分離抽出し,これを用いて活性種及び不活性種の金属酸化物光触媒中での空間分布を得ることが可能になった.

Current Status of Research Progress
Current Status of Research Progress

2: Research has progressed on the whole more than it was originally planned.

Reason

今年度もイタリア側チームと連携をとりながら効率よく研究を進めた.イタリア側はイオンビーム照射による半導体光触媒への不純物元素の添加を担当し,日本側は,若手研究者を中心に電子顕微鏡を用いたEELS測定に着手し,エネルギー分解能の違いはあるもののEELSはXAFSと同等の微細構造を有するスペクトルを与えること,即ち,測定の基本コンセプトを確認した.これを踏まえて,金属酸化物光触媒に対してイオン注入法により光触媒表面に窒素などのアニオン種を添加し,このアニオン種を対象としたELNESスペクトルと表面敏感測定法により取得したXANESスペクトルの比較と化学状態解析をイタリア側と日本側が議論しながら効率的に進めることができたことから,概ね順調に実施できていると判断した.

Strategy for Future Research Activity

イオン注入法の特徴を積極的に利用すると,光触媒に添加する不純物イオンの加速エネルギーを制御することで,光触媒中の目的とする深さ領域に,濃度勾配をつけて中に有することができる.このことから今後の研究においては,可視光照射下での触媒反応活性と,不純物イオンの化学状態や濃度を比較することによって,可視光応答化などの機能を発現させるうえでの最適な不純物イオン濃度や,最適な添加深さ領域に関する知見を得ることを考えている.その際に,イタリア側が得意とする不純物イオンの深さや濃度分布シミュレーション技術も導入し,実験結果に対する理論的解釈も進めたい.

Report

(4 results)
  • 2023 Research-status Report
  • 2022 Research-status Report
  • 2021 Research-status Report
  • 2020 Research-status Report
  • Research Products

    (48 results)

All 2023 2022 2021 2020 2019 Other

All Int'l Joint Research (2 results) Journal Article (18 results) (of which Int'l Joint Research: 1 results,  Peer Reviewed: 18 results,  Open Access: 7 results) Presentation (22 results) (of which Int'l Joint Research: 12 results,  Invited: 9 results) Book (6 results)

  • [Int'l Joint Research] Padova University(イタリア)

    • Related Report
      2021 Research-status Report
  • [Int'l Joint Research] Padova University(イタリア)

    • Related Report
      2020 Research-status Report
  • [Journal Article] Heterogeneous Single-Atom Zinc on Nitrogen-Doped Carbon Catalyzed Electrochemical Allylation of Imines2023

    • Author(s)
      Masuda Ryusuke、Yasukawa Tomohiro、Yamashita Yasuhiro、Maki Tei、Yoshida Tomoko、Kobayashi Shu?
    • Journal Title

      Journal of the American Chemical Society

      Volume: 145 Issue: 22 Pages: 11939-11944

    • DOI

      10.1021/jacs.3c03674

    • Related Report
      2023 Research-status Report
    • Peer Reviewed
  • [Journal Article] 酸化ガリウム光触媒上に担持された銀ナノ粒子のin-situ UV-Vis拡散反射及びXAFS測定2023

    • Author(s)
      山本宗昭、北嶋乃樹、田辺哲朗、吉田朋子
    • Journal Title

      X線分析の進歩

      Volume: 54 Pages: 165-172

    • Related Report
      2023 Research-status Report
    • Peer Reviewed
  • [Journal Article] プラズマ照射によるタングステン材料への光触媒機能付与.2023

    • Author(s)
      吉田朋子、菰口佳吾、小森勝之、梶田信、山本宗昭
    • Journal Title

      X線の進歩

      Volume: 54 Pages: 157-164

    • Related Report
      2023 Research-status Report
    • Peer Reviewed
  • [Journal Article] Effects of Al2O3 and MgAl2O4 Support on Photocatalytic Activity of Ga2O3 in CO2 Reduction with Water2023

    • Author(s)
      Ichikawa Kyoshiro、Aoki Tomomi、Akatsuka Masato、Yamamoto Muneaki、Tanabe Tetsuo、Yoshida Tomoko
    • Journal Title

      Catalysis Letters

      Volume: 154 Issue: 5 Pages: 2008-2022

    • DOI

      10.1007/s10562-023-04424-w

    • Related Report
      2023 Research-status Report
    • Peer Reviewed
  • [Journal Article] Structural and Chemical State Analyses on Nitrided GaOOH as a Visible Light Response Photocatalyst2022

    • Author(s)
      Yamamoto Muneaki、Kato Yuma、Yagi Shinya、Tanabe Tetsuo、Yoshida Tomoko
    • Journal Title

      e-Journal of Surface Science and Nanotechnology

      Volume: 20 Issue: 1 Pages: 1-6

    • DOI

      10.1380/ejssnt.2022-003

    • NAID

      130008158079

    • ISSN
      1348-0391
    • Year and Date
      2022-02-05
    • Related Report
      2022 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Photoelectrochemical properties of plasma-induced nanostructured tungsten oxide2022

    • Author(s)
      Feng Shuangyuan、Kajita Shin、Higashi Masanobu、Bieberle-H?tter Anja、Yoshida Tomoko、Ohno Noriyasu
    • Journal Title

      Applied Surface Science

      Volume: 580 Pages: 151979-151979

    • DOI

      10.1016/j.apsusc.2021.151979

    • Related Report
      2022 Research-status Report 2021 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Mixed phases of GaOOH/α-Ga2O3 and α-Ga2O3/β-Ga2O3 prepared by high energy ball milling as active photocatalysts for CO2 reduction with water2022

    • Author(s)
      T. Aoki, M. Yamamoto, T. Tanabe, T. Yoshida
    • Journal Title

      New J. Chem

      Volume: 46 Issue: 7 Pages: 3207-3213

    • DOI

      10.1039/d1nj05245d

    • Related Report
      2022 Research-status Report 2021 Research-status Report
    • Peer Reviewed
  • [Journal Article] Fabrication of a stable CdS photoanode for photoelectrochemical CO<sub>2</sub> reduction under visible-light irradiation2022

    • Author(s)
      Higashi Masanobu、Tanaka Itsuki、Amao Yutaka、Yoshida Tomoko
    • Journal Title

      New Journal of Chemistry

      Volume: 46 Issue: 13 Pages: 5932-5938

    • DOI

      10.1039/d1nj06073b

    • Related Report
      2022 Research-status Report
    • Peer Reviewed
  • [Journal Article] Synthesis of meso-porous a-Ga2O3 from liquid Ga metal having significantly high photocatalytic activity for CO2 reduction with water2022

    • Author(s)
      T. Aoki, K. Ichikawa, K. Sonoda, M. Yamamoto, T. Tanabe, T. Yoshida
    • Journal Title

      RSC Adv.

      Volume: 12 Issue: 12 Pages: 7164-7167

    • DOI

      10.1039/d1ra09039a

    • Related Report
      2022 Research-status Report 2021 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Synthesis of nanometer-sized gallium oxide using graphene oxide template as a photocatalyst for carbon dioxide reduction2021

    • Author(s)
      K. Sonoda, M. Yamamoto, T. Tanabe, T. Yoshida
    • Journal Title

      Applied Surface Science

      Volume: 542 Pages: 148680

    • DOI

      10.1016/j.apsusc.2020.148680

    • URL

      https://ocu-omu.repo.nii.ac.jp/records/2019637

    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Synthesis of α-Ga<sub>2</sub>O<sub>3</sub> by Water Oxidation of Metallic Gallium as a Photocatalyst for CO<sub>2</sub> Reduction with Water2021

    • Author(s)
      Sonoda Kenta、Yamamoto Muneaki、Tanabe Tetsuo、Yoshida Tomoko
    • Journal Title

      ACS Omega

      Volume: 6 Issue: 29 Pages: 18876-18880

    • DOI

      10.1021/acsomega.1c02088

    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Influence of Ag Clusters on the Electronic Structures of β-Ga<sub>2</sub>O<sub>3</sub> Photocatalyst Surfaces2021

    • Author(s)
      Yamamoto Muneaki、Kuwabara Akihide、Yoshida Tomoko
    • Journal Title

      ACS Omega

      Volume: 6 Issue: 49 Pages: 33701-33707

    • DOI

      10.1021/acsomega.1c04730

    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Real time measurements of UV-vis diffuse reflectance of silver nanoparticles on gallium oxide photocatalyst2021

    • Author(s)
      Kitajima Daiki、Yamamoto Muneaki、Tanabe Tetsuo、Yoshida Tomoko
    • Journal Title

      Catalysis Today

      Volume: 375 Pages: 501-505

    • DOI

      10.1016/j.cattod.2020.04.063

    • URL

      https://ocu-omu.repo.nii.ac.jp/records/2019704

    • Related Report
      2021 Research-status Report
    • Peer Reviewed
  • [Journal Article] Photocatalytic Activity of Metal Oxide Supported Gallium Oxide for CO<sub>2</sub> Reduction with Water2020

    • Author(s)
      Ito Ryota、Akatsuka Masato、Ozawa Akiyo、Yamamoto Muneaki、Tanabe Tetsuo、Yoshida Tomoko
    • Journal Title

      Bulletin of the Chemical Society of Japan

      Volume: 93 Issue: 5 Pages: 694-700

    • DOI

      10.1246/bcsj.20190366

    • NAID

      130007842974

    • ISSN
      0009-2673, 1348-0634
    • Year and Date
      2020-05-15
    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Journal Article] Roles of Silver Co-catalyst on Gallium Oxide for Photocatalytic CO<sub>2</sub> Reduction to CO2020

    • Author(s)
      Yoshioka Kokoro、Yamamoto Muneaki、Tanabe Tetsuo、Yoshida Tomoko
    • Journal Title

      e-Journal of Surface Science and Nanotechnology

      Volume: 18 Issue: 0 Pages: 168-174

    • DOI

      10.1380/ejssnt.2020.168

    • NAID

      130007835843

    • ISSN
      1348-0391
    • Year and Date
      2020-04-25
    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Journal Article] Preparation of Ga2O3 photocatalyst highly active for CO2 reduction with water without cocatalyst2020

    • Author(s)
      M. Akatsuka, Y. Kawaguchi, R. Itoh, A. Ozawa, M. Yamamoto, T. Tanabe, T. Yoshida
    • Journal Title

      Applied Catalysis B: Environmental

      Volume: 262 Pages: 118247-118247

    • DOI

      10.1016/j.apcatb.2019.118247

    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Journal Article] Black phosphorus synthesized by solvothermal reaction from red phosphorus and its catalytic activity for water splitting2020

    • Author(s)
      Ozawa Akiyo、Yamamoto Muneaki、Tanabe Tetsuo、Hosokawa Saburo、Yoshida Tomoko
    • Journal Title

      Journal of Materials Chemistry A

      Volume: 8 Issue: 15 Pages: 7368-7376

    • DOI

      10.1039/c9ta13441g

    • NAID

      120007034008

    • URL

      https://ocu-omu.repo.nii.ac.jp/records/2019998

    • Related Report
      2020 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Effects of the amount of Au nanoparticles on the visible light response of TiO2 photocatalysts2019

    • Author(s)
      Tomoko Yoshida, Yuhei Misu, Muneaki Yamamoto, Tetsuo Tanabe, Jun Kumagai, Satoshi Ogawa, Shinya Yagi
    • Journal Title

      Catalysis Today

      Volume: - Pages: 34-38

    • DOI

      10.1016/j.cattod.2019.12.035

    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Presentation] 総論・ケーススタディ(招待講演)2023

    • Author(s)
      吉田朋子
    • Organizer
      触媒学会
    • Related Report
      2023 Research-status Report
    • Invited
  • [Presentation] イオン注入法による半導体材料への 機能付与2023

    • Author(s)
      山本宗昭、田辺哲朗、吉田朋子
    • Organizer
      X線分析討論会
    • Related Report
      2023 Research-status Report
  • [Presentation] X線吸収分光を基軸とした定量的局所構造・電子状態解析法の構築と複合型その場分析への展開2023

    • Author(s)
      吉田朋子
    • Organizer
      日本分析化学会
    • Related Report
      2023 Research-status Report
    • Invited
  • [Presentation] NITROGEN DOPING INTO THICKNESS-CONTROLLED TITANIUM DIOXIDE PHOTOCATALYSTS2023

    • Author(s)
      Tomoko Yoshida, Tetsuo Tanabe, Muneaki Yamamoto
    • Organizer
      13th International Symposium on "Scientific Bases for the Preparation of Heterogeneous Catalysts"
    • Related Report
      2023 Research-status Report
    • Int'l Joint Research
  • [Presentation] プラズマ駆動型化学反応系の複合分析と機能材料の開拓2023

    • Author(s)
      吉田朋子
    • Organizer
      第70回応用物理学会春季学術講演会
    • Related Report
      2022 Research-status Report
    • Invited
  • [Presentation] Heプラズマ照射タングステン材料の光触媒への応用2022

    • Author(s)
      吉田朋子
    • Organizer
      2022年度ナノ構造触媒研究会講演会
    • Related Report
      2022 Research-status Report
  • [Presentation] The role of Ag-NPs loaded on Ga2O3 on the photocatalytic CO2 reduction studied by in situ spectroscopies2022

    • Author(s)
      M. Yamamoto, T. Yoshida, T. Tanabe
    • Organizer
      14th International Symposium on Atomic Level Characterizations for New Materials and Devices '22
    • Related Report
      2022 Research-status Report
    • Int'l Joint Research
  • [Presentation] プラズマ照射によるタングステン材料への光触媒機能付与2022

    • Author(s)
      山本宗昭,小森勝之,八木伸也,吉田朋子
    • Organizer
      第58回X線分析討論会
    • Related Report
      2022 Research-status Report
  • [Presentation] Characterization of nitrogen doped TiO2 photocatalysts by X-ray absorption and photoemission spectroscopies2022

    • Author(s)
      T. Yoshida, T. Tanabe, S. Yagi, M. Yamamoto
    • Organizer
      14th International Symposium on Atomic Level Characterizations for New Materials and Devices '22
    • Related Report
      2022 Research-status Report
    • Int'l Joint Research
  • [Presentation] Generation of visible light response photocatalysis by nitrogen doping into metal oxides2022

    • Author(s)
      T. Yoshida, Y. Kato, A. Ozawa, T, Tanabe, M. Yamamoto
    • Organizer
      第32回日本MRS年次大会
    • Related Report
      2022 Research-status Report
    • Invited
  • [Presentation] Improvement of photocatalytic activity of Ga2O3 by applying high energy ball milling2021

    • Author(s)
      T. Aoki, R. Ito, K. Sonoda, M. Akatsuka, M. Yamamoto, T. Tanabe, T. Yoshida
    • Organizer
      The international Chemical Congress of Pacific Basin Societies
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research
  • [Presentation] Application of soft X-ray spectroscopy to chemical state analysis of nitrogendoped TiO2 photocatalyst2021

    • Author(s)
      T. Yoshida, A. Ozawa, T. Tanabe, S. Yagi, M. Yamamoto
    • Organizer
      The international Chemical Congress of Pacific Basin Societies
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Fabrication of metal sulfide photoanodes for CO2 reduction under visible ligh2021

    • Author(s)
      I. Tanaka, T. Yoshida, M. Higashi
    • Organizer
      The international Chemical Congress of Pacific Basin Societies
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research
  • [Presentation] Surface modification effects of gallium oxide photocatalyst for carbon dioxide reduction2021

    • Author(s)
      T. Yoshida, M. Akatsuka, R. Ito, K. Yoshioka, T. Tanabe, M. Yamamoto
    • Organizer
      The international Chemical Congress of Pacific Basin Societies
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Application of nitrogen doping to the fabrication of visible light response metal oxide photocatalysts2021

    • Author(s)
      M. Yamamoto, Y. Kato, T. Tanabe, T. Yoshida
    • Organizer
      International Conference on Mixed-Anion Compounds
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research
  • [Presentation] Fabrication of CdS photoanodes for CO2 reduction under visible light2021

    • Author(s)
      I. Tanaka, T. Yoshida, M. Higashi
    • Organizer
      13th International Symposium on Atomic level characterizations for New Materials and Devices ’21
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research
  • [Presentation] Structural modification of β-Ga2O3 to improve the photocatalytic activity for CO2 reduction2021

    • Author(s)
      T. Aoki, M. Yamamoto, T. Tanabe, T. Yoshida
    • Organizer
      13th International Symposium on Atomic level characterizations for New Materials and Devices ’21
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research
  • [Presentation] Chemical state analysis of Ag loaded Ga2O3 as a CO2 reduction photocatalyst2021

    • Author(s)
      M. Yamamoto, T. Tanabe, S. Yagi, T. Yoshida
    • Organizer
      13th International Symposium on Atomic level characterizations for New Materials and Devices ’21
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research
  • [Presentation] Application of nitrogen ion implantation to visible light response of TiO2 photocatalyst2021

    • Author(s)
      T. Yoshida, A. Ozawa, M. Yamamoto, T. Tanabe
    • Organizer
      13th International Symposium on Advanced Plasma Science and its Applications for Nitrides and Nanomaterials
    • Related Report
      2020 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] 金属酸化物光触媒への窒素添加による可視光応答化2020

    • Author(s)
      吉田朋子
    • Organizer
      電気学会
    • Related Report
      2020 Research-status Report
  • [Presentation] 総論・ケーススタディ2020

    • Author(s)
      吉田朋子
    • Organizer
      近畿化学協会
    • Related Report
      2020 Research-status Report
    • Invited
  • [Presentation] X線吸収分光(XAFS)を利用した機能性固体材料のキャラクタリゼーション2020

    • Author(s)
      吉田朋子
    • Organizer
      X線分析研究懇談会
    • Related Report
      2020 Research-status Report
    • Invited
  • [Book] 触媒総合辞典2023

    • Author(s)
      吉田朋子、山本宗昭
    • Total Pages
      4
    • Publisher
      朝倉書店
    • Related Report
      2023 Research-status Report
  • [Book] 触媒総合事典2023

    • Author(s)
      触媒学会
    • Total Pages
      544
    • Publisher
      朝倉書店
    • ISBN
      9784254252743
    • Related Report
      2022 Research-status Report
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Published: 2020-10-29   Modified: 2024-12-25  

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