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2018 Fiscal Year Annual Research Report

Development and activation of stand-alone photocatalyst systems for visible-light-driven water splitting

Research Project

Project/Area Number 15H05494
Research InstitutionShinshu University

Principal Investigator

久富 隆史  信州大学, 先鋭領域融合研究群環境・エネルギー材料科学研究所, 准教授(特定雇用) (00637481)

Project Period (FY) 2015-04-01 – 2019-03-31
Keywords粉末光触媒 / 水分解 / 太陽エネルギー / 水素 / 半導体 / 光触媒シート / Zスキーム / 耐久性
Outline of Annual Research Achievements

本研究は自立型水分解用光触媒反応系として,水素生成光触媒と酸素生成光触媒が導電層に固定化された光触媒シートを作製し,太陽光水素エネルギー変換効率(STH)を向上させることを目指している.平成29年度は水素生成光触媒として710 nmまで長波長側の光を利用可能なLa5Ti2Cu0.9Ag0.1S5O7(LTCA)をZスキーム型光触媒シートに応用可能としたが,酸素生成光触媒には520 nmまでの光しか利用できないBiVO4を用いていた.また,ロジウムクロム複合酸化物助触媒を担持したAlドープSrTiO3(RhCrOx/SrTiO3:Al)にCo種を光電着担持することで,常圧下における水分解活性の耐久性が改善されていたが,1か月程度の反応期間中に活性劣化が見られていた.平成30年度はこれらの課題を克服する成果が得られた.
LaTiO2N光触媒はAuなどの高仕事関数の金属を裏面導電層に用いると活性が著しく悪化するが,予め酸化コバルト種を担持しておくことで光アノード応答が改善されることが見出された.この結果,吸収端波長が710 nm,600 nmとそれぞれ長波長域にあるLTCAとLaTiO2Nを金薄膜に固定化した光触媒シートを用いてZスキーム型水分解反応を駆動させることが可能になった.
RhCrOx/SrTiO3:Al光触媒上にCo種はCoOOHとして酸化的に光電着されていることをオペランドXAFSを用いて明らかにし,CoOOHが正孔を捕捉してCr種の酸化溶出を抑制するために活性劣化が抑制される機構を提示した.さらに,CoOOHとRhCrOxを共担持したSrTiO3:Alに対してTiO2を光電着担持すると,水分解反応活性がより一層安定化することを見出した.1300時間の連続光照射下で初期の活性の8割を維持する光触媒シートを人工光合成プロセス技術検討組合と共同で開発した.

Research Progress Status

平成30年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

平成30年度が最終年度であるため、記入しない。

  • Research Products

    (33 results)

All 2019 2018 Other

All Int'l Joint Research (3 results) Journal Article (16 results) (of which Int'l Joint Research: 4 results,  Peer Reviewed: 16 results,  Open Access: 5 results) Presentation (9 results) (of which Int'l Joint Research: 5 results,  Invited: 8 results) Book (1 results) Remarks (1 results) Patent(Industrial Property Rights) (3 results)

  • [Int'l Joint Research] University of Cambridge/Imperial College London(英国)

    • Country Name
      UNITED KINGDOM
    • Counterpart Institution
      University of Cambridge/Imperial College London
  • [Int'l Joint Research] Univ. Sci. Tech. China/Anhui University(中国)

    • Country Name
      CHINA
    • Counterpart Institution
      Univ. Sci. Tech. China/Anhui University
  • [Int'l Joint Research] National United University, Taiwan(その他の国・地域)

    • Country Name
      その他の国・地域
    • Counterpart Institution
      National United University, Taiwan
  • [Journal Article] Revealing the role of the Rh valence state, La doping level and Ru cocatalyst in determining the H2 evolution efficiency in doped SrTiO3 photocatalysts2019

    • Author(s)
      Murthy Dharmapura H. K.、Matsuzaki Hiroyuki、Wang Qian、Suzuki Yohichi、Seki Kazuhiko、Hisatomi Takashi、Yamada Taro、Kudo Akihiko、Domen Kazunari、Furube Akihiro
    • Journal Title

      Sustainable Energy & Fuels

      Volume: 3 Pages: 208~218

    • DOI

      10.1039/C8SE00487K

    • Peer Reviewed
  • [Journal Article] Regression model for stabilization energies associated with anion ordering in perovskite-type oxynitrides2019

    • Author(s)
      Kaneko Masanori、Fujii Mikiya、Hisatomi Takashi、Yamashita Koichi、Domen Kazunari
    • Journal Title

      Journal of Energy Chemistry

      Volume: 36 Pages: 7~14

    • DOI

      10.1016/j.jechem.2019.01.012

    • Peer Reviewed
  • [Journal Article] Visible‐Light‐Driven Photocatalytic Z‐Scheme Overall Water Splitting in La5Ti2AgS5O7‐based Powder‐Suspension System2019

    • Author(s)
      Song Zhimin、Hisatomi Takashi、Chen Shanshan、Wang Qian、Ma Guijun、Li Shikuo、Zhu Xiaodi、Sun Song、Domen Kazunari
    • Journal Title

      ChemSusChem

      Volume: 12 Pages: 1906~1910

    • DOI

      10.1002/cssc.201802306

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] An Al-doped SrTiO3 photocatalyst maintaining sunlight-driven overall water splitting activity for over 1000 h of constant illumination2019

    • Author(s)
      Lyu Hao、Hisatomi Takashi、Goto Yosuke、Yoshida Masaaki、Higashi Tomohiro、Katayama Masao、Takata Tsuyoshi、Minegishi Tsutomu、Nishiyama Hiroshi、Yamada Taro、Sakata Yoshihisa、Asakura Kiyotaka、Domen Kazunari
    • Journal Title

      Chemical Science

      Volume: 10 Pages: 3196~3201

    • DOI

      DOI: 10.1039/c8sc05757e

    • Peer Reviewed / Open Access
  • [Journal Article] Metal Selenides for Photocatalytic Z-scheme Pure Water Splitting Mediated by Reduced Graphene Oxide2019

    • Author(s)
      Shanshan Chen, Takashi Hisatomi, Guijun Ma, Zheng Wang, Zhenhua Pan, Tsuyoshi Takata, Kazunari Domen
    • Journal Title

      Chinese Journal of Catalysis

      Volume: 印刷中 Pages: -

    • Peer Reviewed
  • [Journal Article] Metal selenide photocatalysts for visible-light-driven Z-scheme pure water splitting2019

    • Author(s)
      Chen Shanshan、Ma Guijun、Wang Qian、Sun Song、Hisatomi Takashi、Higashi Tomohiro、Wang Zheng、Nakabayashi Mamiko、Shibata Naoya、Pan Zhenhua、Hayashi Toshio、Minegishi Tsutomu、Takata Tsuyoshi、Domen Kazunari
    • Journal Title

      Journal of Materials Chemistry A

      Volume: 7 Pages: 7415~7422

    • DOI

      DOI: 10.1039/C9TA00768G

    • Peer Reviewed / Open Access
  • [Journal Article] Reaction systems for solar hydrogen production via water splitting with particulate semiconductor photocatalysts2019

    • Author(s)
      Hisatomi Takashi、Domen Kazunari
    • Journal Title

      Nature Catalysis

      Volume: 2 Pages: 387~399

    • DOI

      10.1038/s41929-019-0242-6

    • Peer Reviewed
  • [Journal Article] La5Ti2Cu0.9Ag0.1S5O7 Modified with a Molecular Ni Catalyst for Photoelectrochemical H2 Generation2018

    • Author(s)
      Rosser Timothy E.、Hisatomi Takashi、Sun Song、Daniel Anton-Garcia、Minegishi Tsutomu、Reisner Erwin、Domen Kazunari
    • Journal Title

      Chemistry - A European Journal

      Volume: 24 Pages: 18393~18397

    • DOI

      DOI:10.1002/chem.201801169

    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Effects of Se Incorporation in La5Ti2CuS5O7 by Annealing on Physical Properties and Photocatalytic H2 Evolution Activity2018

    • Author(s)
      Nandy Swarnava、Hisatomi Takashi、Sun Song、Katayama Masao、Minegishi Tsutomu、Domen Kazunari
    • Journal Title

      ACS Applied Materials & Interfaces

      Volume: 11 Pages: 5595~5601

    • DOI

      DOI: 10.1021/acsami.8b02909

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Direct observation of hydrogen bubble generation on photocatalyst particles by in situ electron microscopy2018

    • Author(s)
      Daio Takeshi、Narita Ichihito、Nandy Swarnava、Hisatomi Takashi、Domen Kazunari、Suganuma Katsuaki
    • Journal Title

      Chemical Physics Letters

      Volume: 706 Pages: 564~567

    • DOI

      10.1016/j.cplett.2018.05.081

    • Peer Reviewed
  • [Journal Article] Particulate photocatalyst sheets based on non-oxide semiconductor materials for water splitting under visible light irradiation2018

    • Author(s)
      Hisatomi Takashi、Yamamoto Takahiro、Wang Qian、Nakanishi Takahiro、Higashi Tomohiro、Katayama Masao、Minegishi Tsutomu、Domen Kazunari
    • Journal Title

      Catalysis Science & Technology

      Volume: 8 Pages: 3918~3925

    • DOI

      10.1039/C8CY00860D

    • Peer Reviewed
  • [Journal Article] Overall water splitting by Ta3N5 nanorod single crystals grown on the edges of KTaO3 particles2018

    • Author(s)
      Wang Zheng、Inoue Yasunobu、Hisatomi Takashi、Ishikawa Ryo、Wang Qian、Takata Tsuyoshi、Chen Shanshan、Shibata Naoya、Ikuhara Yuichi、Domen Kazunari
    • Journal Title

      Nature Catalysis

      Volume: 1 Pages: 756~763

    • DOI

      10.1038/s41929-018-0134-1

    • Peer Reviewed
  • [Journal Article] Understanding the visible-light photocatalytic activity of GaN:ZnO solid solution: the role of Rh2-yCryO3 cocatalyst and charge carrier lifetimes over tens of seconds2018

    • Author(s)
      Godin Robert、Hisatomi Takashi、Domen Kazunari、Durrant James R.
    • Journal Title

      Chemical Science

      Volume: 9 Pages: 7546~7555

    • DOI

      10.1039/C8SC02348D

    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Printable Photocatalyst Sheets Incorporating a Transparent Conductive Mediator for Z-Scheme Water Splitting2018

    • Author(s)
      Wang Qian、Okunaka Sayuri、Tokudome Hiromasa、Hisatomi Takashi、Nakabayashi Mamiko、Shibata Naoya、Yamada Taro、Domen Kazunari
    • Journal Title

      Joule

      Volume: 2 Pages: 2667~2680

    • DOI

      10.1016/j.joule.2018.08.003

    • Peer Reviewed
  • [Journal Article] Investigation on nitridation processes of Sr2Nb2O7 and SrNbO3 to SrNbO2N for photoelectrochemical water splitting2018

    • Author(s)
      Kodera Masanori、Moriya Yosuke、Katayama Masao、Hisatomi Takashi、Minegishi Tsutomu、Domen Kazunari
    • Journal Title

      Scientific Reports

      Volume: 8 Pages: 15849

    • DOI

      10.1038/s41598-018-34184-2

    • Peer Reviewed / Open Access
  • [Journal Article] Effects of annealing conditions on the oxygen evolution activity of a BaTaO2N photocatalyst loaded with cobalt species2018

    • Author(s)
      Okamoto Hiroya、Kodera Masanori、Hisatomi Takashi、Katayama Masao、Minegishi Tsutomu、Domen Kazunari
    • Journal Title

      Catalysis Today

      Volume: 印刷中 Pages: -

    • DOI

      10.1016/j.cattod.2018.12.048

    • Peer Reviewed
  • [Presentation] Heterogeneous Photocatalysts and Reaction Systems for Renewable Hydrogen Production via Water Splitting2019

    • Author(s)
      Takashi Hisatomi
    • Organizer
      International Symposium on heterogeneous catalysis for sustainable energy and chemical production, Sapporo, Japan
    • Int'l Joint Research / Invited
  • [Presentation] 可視光水分解反応に活性なY2Ti2S2O5光触媒2019

    • Author(s)
      久富隆史,王謙,秋山誠治,山田太郎,高田剛,堂免一成
    • Organizer
      日本化学会第99春季年会
  • [Presentation] Strategies and focuses for photocatalytic and photoelectrochemical H2 production in Japan2018

    • Author(s)
      Takashi Hisatomi, Kazunari Domen
    • Organizer
      PEC Working Group Meeting, Seattle, United States of America
    • Int'l Joint Research / Invited
  • [Presentation] Particulate Photocatalyst Systems for Sunlight-driven Water Splitting2018

    • Author(s)
      Takashi Hisatomi, Kazunari Domen
    • Organizer
      233rd ECS MEETING, Seattle, United States of America
    • Int'l Joint Research / Invited
  • [Presentation] Development of La5Ti2Cu(S1-xSex)5O7 photocatalysts for hydrogen evolution from water under visible light irradiation.2018

    • Author(s)
      Takashi Hisatomi, Swarnava Nandy, Yosuke Goto, Yosuke Moriya, Guijun Ma, Masao Katayama, Tsutomu Minegishi, Kazunari Domen
    • Organizer
      The 8th Tokyo Conference on Advanced Catalytic Science and Technology (TOCAT8), Yokohama, Japan
    • Int'l Joint Research / Invited
  • [Presentation] Operando XAFS measurements of water splitting photocatalysts2018

    • Author(s)
      Takashi Hisatomi, Kazunari Domen
    • Organizer
      The 2018 MRS Fall Meeting & Exhibit, Boston, United States of America
    • Int'l Joint Research / Invited
  • [Presentation] 粉末光触媒を用いた太陽光水分解反応系の構築2018

    • Author(s)
      久富隆史
    • Organizer
      日本セラミックス協会第31回秋季シンポジウム
    • Invited
  • [Presentation] 太陽光水分解反応を目的とした粉末半導体光触媒の開発2018

    • Author(s)
      久富隆史
    • Organizer
      第112回触媒討論会
    • Invited
  • [Presentation] 可視光水分解用粉末光触媒の開発2018

    • Author(s)
      久富隆史
    • Organizer
      第47回結晶成長国内会議
    • Invited
  • [Book] Particulate photocatalyst sheets for efficient and scalable water splitting; in Advances in Photoelectrochemical Water Splitting2018

    • Author(s)
      Takashi Hisatomi, Kazunari Domen
    • Total Pages
      25
    • Publisher
      Royal Society of Chemistry
  • [Remarks] 世界初、太陽の可視光を吸収して水を分解する窒化タンタル光触媒を開発

    • URL

      https://www.nedo.go.jp/news/press/AA5_101014.html

  • [Patent(Industrial Property Rights)] 光触媒と、この光触媒を用いた水素及び酸素の製造方法2019

    • Inventor(s)
      堂免一成,王謙,久富隆史,パクヨハン,秋山誠治,吉田紘章
    • Industrial Property Rights Holder
      東京大学、信州大学、三菱ケミカル、人工光合成化学プロセス技組
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      特願2019-031783
  • [Patent(Industrial Property Rights)] 表面に助触媒を担持した光触媒及び該光触媒の製造方法2019

    • Inventor(s)
      堂免一成,久富隆史,オウセイ,手嶋勝弥,鈴木清香,ロイン,他1名
    • Industrial Property Rights Holder
      信州大学、三菱ケミカル、人工光合成化学プロセス技術研究組合
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      特願2019-041808
  • [Patent(Industrial Property Rights)] 光触媒と、この光触媒を用いた水素及び酸素の製造方法2018

    • Inventor(s)
      堂免一成,王謙,久富隆史,パクヨハン,秋山誠治,吉田紘章
    • Industrial Property Rights Holder
      東京大学、信州大学、三菱ケミカル、人工光合成化学プロセス技組
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      特願2018-173350

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Published: 2019-12-27  

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