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高効率な時間分解XAFS法を用いた光反応中間体の詳細な構造解析

Publicly Offered Research

Project AreaChemical conversion of solar energy by artificial photosynthesis: a breakthrough by fusion of related fields toward realization of practical processes
Project/Area Number 15H00890
Research Category

Grant-in-Aid for Scientific Research on Innovative Areas (Research in a proposed research area)

Allocation TypeSingle-year Grants
Review Section Science and Engineering
Research InstitutionHigh Energy Accelerator Research Organization

Principal Investigator

野澤 俊介  大学共同利用機関法人高エネルギー加速器研究機構, 物質構造科学研究所, 准教授 (20415053)

Project Period (FY) 2015-04-01 – 2017-03-31
Project Status Completed (Fiscal Year 2016)
Budget Amount *help
¥3,640,000 (Direct Cost: ¥2,800,000、Indirect Cost: ¥840,000)
Fiscal Year 2016: ¥1,820,000 (Direct Cost: ¥1,400,000、Indirect Cost: ¥420,000)
Fiscal Year 2015: ¥1,820,000 (Direct Cost: ¥1,400,000、Indirect Cost: ¥420,000)
Keywords人工光合成 / 光機能材料 / 分子動画 / 量子ビーム / 再生可能エネルギー / エネルギー効率化 / X線 / 可視化 / 光物性
Outline of Annual Research Achievements

前年度インストールが完了した高繰り返しファイバーレーザーを用い、X線集光レンズに改良を加えマイクロビーム条件でポンププローブ測定を実施し、高周波数帯における変調法により過渡的なX線シグナルを抽出することにより、放射光施設PF-ARから794kHzで発せられるパルスX線を間引かずに全て利用するピコ秒時間分解XAFSシステムを構築した。ビームラインNW14Aに設置された周期超36mmのアンジュレーターを用いると5-24keVにおいて、広い波数空間においてS/N比の良い過渡EXAFSスペクトルを得ることが可能となり、Ti,Fe,Co,W,Re、Ir,Os,Ru等の光触媒反応に重要な元素周りの局所的な動的構造解析が行えるようになった。
本研究においてまず、測定ターゲットとした選定されたホスフィン配位子の種類を変えたRe(I)錯体の3MLCT状態の動的構造解析では、電荷移動に起因した金属元素周りの構造歪みから、励起状態では配位子間において強いπ-π相互作用が働いており、触媒効率と相関があることが示唆された。
また、Ru(II)錯体の3MLCT状態における、励起状態の電子状態と過渡的な構造変化に関する研究においては、配位子を変えた類似錯体と励起状態の過渡EXAFSスペクトルを比較研究することで、光励起電荷移動によって一つの配位子に電子が局在した過渡的な電子状態変化により、配位子構造の対称性低下が引き起こされていることが明らかになった。

Research Progress Status

28年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

28年度が最終年度であるため、記入しない。

Report

(2 results)
  • 2016 Annual Research Report
  • 2015 Annual Research Report
  • Research Products

    (22 results)

All 2017 2016 2015 Other

All Int'l Joint Research (3 results) Journal Article (7 results) (of which Int'l Joint Research: 2 results,  Peer Reviewed: 7 results,  Acknowledgement Compliant: 5 results,  Open Access: 1 results) Presentation (11 results) (of which Int'l Joint Research: 7 results,  Invited: 6 results) Book (1 results)

  • [Int'l Joint Research] プサン大(韓国)

    • Related Report
      2015 Annual Research Report
  • [Int'l Joint Research] ローレンス・バークレー国立研究所(米国)

    • Related Report
      2015 Annual Research Report
  • [Int'l Joint Research] ドイツ電子シンクロトロン(ドイツ)

    • Related Report
      2015 Annual Research Report
  • [Journal Article] Solar-driven Z-scheme water splitting using tantalum/nitrogen co-doped rutile titania nanorod as an oxygen evolution photocatalyst2017

    • Author(s)
      A. Nakada, S. Nishioka, J. J. M. Vequizo, K. Muraoka, T. Kanazawa A. Yamakata, S. Nozawa, H. Kumagai, S. Adachi, O. Ishitani, K. Maeda
    • Journal Title

      Journal of Materials Chemistry A

      Volume: . Issue: 23 Pages: 11710-11719

    • DOI

      10.1039/c6ta10541f

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Cobalt Oxide Nanoclusters on Rutile Titania as Bifunctional Units for Water Oxidation Catalysis and Visible Light Absorption: Understanding the Structure Activity Relationship2017

    • Author(s)
      K. Maeda, K. Ishimaki, M. Okazaki, T. Kanazawa, D. Lu, S. Nozawa, H. Kato, M. Kakihana
    • Journal Title

      ACS Appl. Mater. Interfaces

      Volume: 9 Issue: 7 Pages: 6114-6122

    • DOI

      10.1021/acsami.6b15804

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] A Ruthenium(III)-Oxyl Complex Bearing Strong Radical Character2016

    • Author(s)
      Y. Shimoyama, T. Ishizuka, H. Kotani, Y. Shiota, K. Yoshizawa, K. Mieda, T. Ogura, T. Okajima, S. Nozawa, T. Kojima
    • Journal Title

      Angewandte Chemie International Edition

      Volume: 55 Issue: 45 Pages: 14041-14045

    • DOI

      10.1002/anie.201607861

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Femtosecond X-ray solution scattering reveals that bond formation mechanism of a gold trimer complex is independent of excitation wavelength2016

    • Author(s)
      K. H. Kim, J. G. Kim, K. Y. Oang, T. W. Kim, H. Ki, J. Jo, J. Kim, T. Sato, S. Nozawa, S. Adachi, H. Ihee
    • Journal Title

      Struct. Dyn.

      Volume: 3 Issue: 4 Pages: 043209-043209

    • DOI

      10.1063/1.4948516

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Int'l Joint Research / Acknowledgement Compliant
  • [Journal Article] Visible-Light-Responsive CuLi1/3Ti2/3O2 Powders Prepared by a Molten CuCl Treatment of Li2TiO3 for Photocatalytic H2 Evolution and Z‐Schematic Water Splitting2016

    • Author(s)
      K. Iwashina, A. Iwase, S. Nozawa, S. Adachi, A. Kudo
    • Journal Title

      Chem. Mater.

      Volume: 28 Issue: 13 Pages: 4677-4685

    • DOI

      10.1021/acs.chemmater.6b01557

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Visualization of the birth of molecules by XFEL2016

    • Author(s)
      S. Nozawa
    • Journal Title

      Japanese Journal of Optics

      Volume: 45 Pages: 432-437

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Dynamics of Photoelectrons and Structural changes of Tungsten Trioxide Observed by Femtosecond Transient XAFS2016

    • Author(s)
      Y. Uemura, D. Kido, Y. Wakisaka, H. Uehara, T. ohba, Y. Niwa, S. Nozawa, T. Sato, K. Ichiyanagi, R. Fulaya, T. Katayama, T. Togashi, S. Owada, M. Yabashi, K. Hatada, S. Takakusagi, T. Yokoyama, B. Ohtani, K. Asakura
    • Journal Title

      Angewandte Chemie International Edition

      Volume: 55 Issue: 4 Pages: 1364-1367

    • DOI

      10.1002/anie.201509252

    • NAID

      120005946855

    • Related Report
      2015 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Presentation] Visualization of transient molecular structures by high-repetition-rate time-resolved XAFS2017

    • Author(s)
      Shunsuke Nozawa
    • Organizer
      2017 International Conference on Artificial Photosynthesis
    • Place of Presentation
      立命館大学(滋賀県・草津市)
    • Year and Date
      2017-03-02
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Direct observation of bond formation by femtosecond X-ray solution scattering2016

    • Author(s)
      Shunsuke Nozawa, Kyung Hwan Kim, Jong Goo Kim, Tokushi Sato,Key Young Oang, Tae Wu Kim, Hosung Ki, Junbeom Jo, Sungjun Park, Changyong Song, Takahiro Sato, Kanade Ogawa, Tadashi Togashi, Kensuke Tono, Makina Yabashi, Tetsuya Ishikawa, Joonghan Kim, Ryong Ryoo, Jeongho Kim Hyotcherl Ihee, Shin-ichi Adachi
    • Organizer
      2016 Asian Crystallographic Association Meeting
    • Place of Presentation
      ベトナム, ハノイ, Hanoi University of Science and Technology
    • Year and Date
      2016-12-04
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Upgrade the beamline PF-AR NW14A for the high-reptitionrate x-ray pump-probe experiments2016

    • Author(s)
      野澤俊介
    • Organizer
      9th edition of the Mechanical Engineering Design of Synchrotron Radiation Equipment and Instrumentation (MEDSI) conference
    • Place of Presentation
      スペイン, バルセロナ, Cosmocaixa, the science museum of Barcelona
    • Year and Date
      2016-09-11
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research
  • [Presentation] PF-AR NW14Aで再構築された高繰り返しピコ秒時間分解XAFS2016

    • Author(s)
      野澤俊介
    • Organizer
      第19回XAFS討論会
    • Place of Presentation
      名古屋大学(愛知県・名古屋市)
    • Year and Date
      2016-09-03
    • Related Report
      2016 Annual Research Report
  • [Presentation] Ultrafast molecular structural dynamics of metal complexes probed by time-resolved X-ray experiments2015

    • Author(s)
      Shunsuke Nozawa
    • Organizer
      Pacifichem2015
    • Place of Presentation
      ホノルル(アメリカ)
    • Year and Date
      2015-12-15
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] フェムト秒 X 線溶液散乱による化学結合形成に伴った分子生成過程の可視化2015

    • Author(s)
      野澤俊介
    • Organizer
      東北大学金属材料研究所研究会 「量子ビーム強磁場実験の進展と将来-基礎物理および物質科学への応用」
    • Place of Presentation
      東北大学金属材料研究所(岩手県・仙台市)
    • Year and Date
      2015-09-30
    • Related Report
      2015 Annual Research Report
    • Invited
  • [Presentation] Excited-state Molecular Structures of Metal Complexes Measured by Time-resolved XAFS2015

    • Author(s)
      Shunsuke Nozawa
    • Organizer
      XAFS16
    • Place of Presentation
      カールスルーエ(ドイツ)
    • Year and Date
      2015-08-23
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research
  • [Presentation] X 線自由電子レーザー(XFEL)を用いたフェムト秒分子動画撮影法による化学結合形成に伴った分子生成過程の可視化2015

    • Author(s)
      野澤俊介
    • Organizer
      第27回 配位化合物の光化学討論会
    • Place of Presentation
      佐渡インフォメーションセンター(新潟県・佐渡市)
    • Year and Date
      2015-08-07
    • Related Report
      2015 Annual Research Report
  • [Presentation] Molecular Structural Dynamics of Photofunctional Complexes Probed by Time-resolved XAFS and X-ray Liquid Scattering2015

    • Author(s)
      Shunsuke Nozawa
    • Organizer
      IUPAC-2015
    • Place of Presentation
      プサン(韓国)
    • Year and Date
      2015-08-06
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 太陽電池や光触媒の基礎反応である電子移動のメカニズム2015

    • Author(s)
      野澤俊介
    • Organizer
      第18回 XAFS討論会
    • Place of Presentation
      高エネルギー加速器研究機構(茨城県・つくば市)
    • Year and Date
      2015-07-29
    • Related Report
      2015 Annual Research Report
    • Invited
  • [Presentation] Direct observation of bond formation by femtosecond X-ray solution scattering2015

    • Author(s)
      Shunsuke Nozawa
    • Organizer
      SRI2015
    • Place of Presentation
      ニューヨーク(アメリカ)
    • Year and Date
      2015-07-06
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research / Invited
  • [Book] 産業応用を目指した無機・有機新材料創製のための構造解析技術2015

    • Author(s)
      一柳光平, 野澤俊介
    • Total Pages
      19
    • Publisher
      CMC出版
    • Related Report
      2015 Annual Research Report

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Published: 2015-04-16   Modified: 2022-01-27  

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