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Development of operando PTRF-XAFS technique and its application to 3D structure analysis of catalyst active sites under working conditions

Research Project

Project/Area Number 18H01864
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Review Section Basic Section 29020:Thin film/surface and interfacial physical properties-related
Research InstitutionHokkaido University

Principal Investigator

Takakusagi Satoru  北海道大学, 触媒科学研究所, 准教授 (30359484)

Project Period (FY) 2018-04-01 – 2021-03-31
Project Status Completed (Fiscal Year 2020)
Budget Amount *help
¥17,420,000 (Direct Cost: ¥13,400,000、Indirect Cost: ¥4,020,000)
Fiscal Year 2020: ¥4,680,000 (Direct Cost: ¥3,600,000、Indirect Cost: ¥1,080,000)
Fiscal Year 2019: ¥4,680,000 (Direct Cost: ¥3,600,000、Indirect Cost: ¥1,080,000)
Fiscal Year 2018: ¥8,060,000 (Direct Cost: ¥6,200,000、Indirect Cost: ¥1,860,000)
Keywordsオペランド偏光全反射蛍光XAFS法 / 担持金属触媒 / 三次元構造解析 / 担体効果 / 偏光全反射蛍光XAFS法
Outline of Final Research Achievements

Oxide-supported metal catalysts are widely used as practical catalysts. It is indispensable to reveal electronic states and 3D structures of the active metal species during catalytic reactions for atomic-level understanding of the relationships between catalyst structure and activity, and also for further development of high-performance catalysts. We have succeeded in constructing operando polarization-dependent total reflection fluorescence XAFS (PTRF-XAFS) technique which can obtain information on electronic state (XANES) and 3D structure (EXAFS) of highly dispersed metal species on an oxide single-crystal support surface by upgrading our previously developed ultra-high vacuum (UHV) PTRF-XAFS technique. We applied this novel operando PTRF-XAFS technique to CO oxidation on a Pt/Al2O3(0001) model catalyst surface and performed analysis of electronic state and 3D structure of the active Pt sites.

Academic Significance and Societal Importance of the Research Achievements

触媒(固体触媒)はファインケミカルズや医薬品の合成、自動車排ガスの無害化など、産業や環境に有用な多くの化学反応に用いられている。持続可能な社会の実現には、触媒の更なる高性能化(高活性・高選択性)が求められる。しかし、“触媒反応中にどういった電子状態及び三次元構造を有する表面ナノ構造が形成され、活性サイトとして機能しているのか?”に関する情報は、評価技術が十分に確立されておらず多くの場合不明であり、高性能触媒実現のための設計指針を得ることが難しかった。本研究で開発したオペランド偏光全反射蛍光XAFS法はこうした情報の取得を可能とし、今後の高性能触媒設計に関して明確な指針を提示できると期待される。

Report

(4 results)
  • 2020 Annual Research Report   Final Research Report ( PDF )
  • 2019 Annual Research Report
  • 2018 Annual Research Report
  • Research Products

    (36 results)

All 2021 2020 2019 2018 Other

All Journal Article (17 results) (of which Int'l Joint Research: 3 results,  Peer Reviewed: 17 results,  Open Access: 3 results) Presentation (16 results) (of which Int'l Joint Research: 7 results,  Invited: 11 results) Remarks (3 results)

  • [Journal Article] Thorough Search Analysis of Extended X-ray Absorption Fine Structure Data for Complex Molecules and Nanomaterials Applications2020

    • Author(s)
      Kido Daiki、Uemura Yohei、Wakisaka Yuki、Ariga-Miwa Hiroko、Takakuasgi Satoru、Asakura Kiyotaka
    • Journal Title

      e-Journal of Surface Science and Nanotechnology

      Volume: 18 Issue: 0 Pages: 249-261

    • DOI

      10.1380/ejssnt.2020.249

    • NAID

      130007883913

    • ISSN
      1348-0391
    • Year and Date
      2020-08-01
    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Operando Observations of a Manganese Oxide Electrocatalyst for Water Oxidation Using Hard/Tender/Soft X-ray Absorption Spectroscopy2020

    • Author(s)
      Shun Tsunekawa, Futaba Yamamoto, Ke-Hsuan Wang, Masanari Nagasaka, Hayato Yuzawa, Satoru Takakusagi, Hiroshi Kondoh, Kiyotaka Asakura, Takeshi Kawai, and Masaaki Yoshida
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 124 Issue: 43 Pages: 23611-23618

    • DOI

      10.1021/acs.jpcc.0c05571

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Bent crystal Laue analyser combined with total reflection fluorescence X-ray absorption fine structure (BCLA + TRF-XAFS) and its application to surface studies2020

    • Author(s)
      Wakisaka Yuki、Hu Bing、Kido Daiki、Al Rashid Md. Harun、Chen Wenhan、Dong Kaiyue、Wada Takahiro、Bharate Bapurao、Yuan Quiyi、Mukai Shingo、Takeichi Yasuo、Takakusagi Satoru、Asakura Kiyotaka
    • Journal Title

      Journal of Synchrotron Radiation

      Volume: 27 Issue: 6 Pages: 1618-1625

    • DOI

      10.1107/s1600577520011170

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Transfer hydrogenolysis of aromatic ethers promoted by the bimetallic Pd/Co catalyst2019

    • Author(s)
      F.Mauriello, H.Ariga-Miwa,PaoneaR.Pietropaolo, S.Takakusagi, K.Asakura
    • Journal Title

      Catalysis Today

      Volume: - Pages: 511-517

    • DOI

      10.1016/j.cattod.2019.06.071

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Statistical Analysis and Discovery of Heterogeneous Catalysts Based on Machine Learning from Diverse Published Data2019

    • Author(s)
      Suzuki Keisuke、Toyao Takashi、Maeno Zen、Takakusagi Satoru、Shimizu Ken‐ichi、Takigawa Ichigaku
    • Journal Title

      ChemCatChem

      Volume: 11 Issue: 18 Pages: 4537-4547

    • DOI

      10.1002/cctc.201900971

    • NAID

      120006866531

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Metamorphosis-like Transformation during Activation of In/SiO2 Catalyst for Non-oxidative Coupling of Methane: In Situ X-ray Absorption Fine Structure Analysis2019

    • Author(s)
      Kashaboina Upendar、Nishikawa Yuta、Wakisaka Yuki、Sirisit Natee、Nagamatsu Shin-ichi、Bao Deling、Ariga-Miwa Hiroko、Takakusagi Satoru、Inami Yuta、Kuriyama Fumiya、Dipu Arnoldus Lambertus、Ogihara Hitoshi、Iguchi Shoji、Yamanaka Ichiro、Wada Takahiro、Asakura Kiyotaka
    • Journal Title

      Chemistry Letters

      Volume: 48 Issue: 9 Pages: 1145-1147

    • DOI

      10.1246/cl.190440

    • NAID

      130007703042

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Linear Correlations between Adsorption Energies and HOMO Levels for the Adsorption of Small Molecules on TiO2 Surfaces2019

    • Author(s)
      Kamachi Takashi、Tatsumi Toshinobu、Toyao Takashi、Hinuma Yoyo、Maeno Zen、Takakusagi Satoru、Furukawa Shinya、Takigawa Ichigaku、Shimizu Ken-ichi
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 123 Issue: 34 Pages: 20988-20997

    • DOI

      10.1021/acs.jpcc.9b05707

    • NAID

      120006882088

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Machine Learning for Catalysis Informatics: Recent Applications and Prospects2019

    • Author(s)
      Toyao Takashi、Maeno Zen、Takakusagi Satoru、Kamachi Takashi、Takigawa Ichigaku、Shimizu Ken-ichi
    • Journal Title

      ACS Catalysis

      Volume: 10 Issue: 3 Pages: 2260-2297

    • DOI

      10.1021/acscatal.9b04186

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Photoinduced anisotropic distortion as the electron trapping site of tungsten trioxide by ultrafast W L1-edge X-ray absorption spectroscopy with full potential multiple scattering calculations2019

    • Author(s)
      Koide Akihiro, Hatada Keisuke et al.
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 19 Issue: 5 Pages: 1-7

    • DOI

      10.1039/c9cp01332f

    • NAID

      120006957263

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Evidence for Multi-Atom Resonance X-ray Raman Spectroscopy &mdash; An <i>in situ</i> Low <i>Z</i>-element and Bond-specific X-ray Spectroscopy2018

    • Author(s)
      Sirisit Natee、Kido Daiki、Wakisaka Yuki、Ariga-Miwa Hiroko、Takakusagi Satoru、Asakura Kiyotaka、Sekizawa Oki、Sakata Tomohiro、Uruga Tomoya、Iwasawa Yasuhiro
    • Journal Title

      e-Journal of Surface Science and Nanotechnology

      Volume: 16 Issue: 0 Pages: 387-390

    • DOI

      10.1380/ejssnt.2018.387

    • NAID

      130007480043

    • ISSN
      1348-0391
    • Year and Date
      2018-09-01
    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Ultra-high Dispersion of Metals on an Oxide Single-crystal Surface Premodified with a Functional Organic Molecule and Their 3D Structure Analysis by PTRF-XAFS Technique2018

    • Author(s)
      TAKAKUSAGI Satoru、ASAKURA Kiyotaka
    • Journal Title

      Vacuum and Surface Science

      Volume: 61 Issue: 5 Pages: 309-314

    • DOI

      10.1380/vss.61.309

    • NAID

      130006733720

    • ISSN
      2433-5835, 2433-5843
    • Year and Date
      2018-05-10
    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Toward effective utilization of methane: machine learning prediction of adsorption energies on metal alloys2018

    • Author(s)
      Toyao T, Suzuki K, Kikuchi S, Takakusagi S, Shimizu K, Takigawa I
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 122 (15) Issue: 15 Pages: 8315-8326

    • DOI

      10.1021/acs.jpcc.7b12670

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] A Demonstration of Pt L3-Edge EXAFS Free from Au L3-Edge Using Log-Spiral Bent Crystal Laue Analyzers2018

    • Author(s)
      Wakisaka Yuki、Kido Daiki、Uehara Hiromitsu、Yuan Qiuyi、Takakusagi Satoru、Uemura Yohei、Yokoyama Toshihiko、Wada Takahiro、Uo Motohiro、Sakata Tomohiro、Sekizawa Oki、Uruga Tomoya、Iwasawa Yasuhiro、Asakura Kiyotaka
    • Journal Title

      Catalysts

      Volume: 8 Issue: 5 Pages: 204-204

    • DOI

      10.3390/catal8050204

    • NAID

      120006491529

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Incorporation of Multinuclear Copper Active Sites into Nitrogen-Doped Graphene for Electrochemical Oxygen Reduction2018

    • Author(s)
      Masaru Kato, Marika Muto, Naohiro Matsubara, Yohei Uemura, Yuki Wakisaka, Tsubasa Yoneuchi, Daiju Matsumura, Tomoko Ishihara, Takashi Tokushima, Shin-ichiro Noro, Satoru Takakusagi, Kiyotaka Asakura, and Ichizo Yagi
    • Journal Title

      ACS Appl. Energy Mater.

      Volume: 1 Issue: 5 Pages: 2358-2364

    • DOI

      10.1021/acsaem.8b00491

    • NAID

      120006887744

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Reaction Stoichiometry and Mechanism of Pt Deposition via Surface Limited Redox Replacement of Copper UPD Layer on Au(111)2018

    • Author(s)
      Yuan Qiuyi、Wakisaka Yuki、Uemura Yohei、Wada Takahiro、Ariga-Miwa Hiroko、Takakusagi Satoru、Asakura Kiyotaka、Brankovic Stanko R.
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 122 Issue: 29 Pages: 16664-16673

    • DOI

      10.1021/acs.jpcc.8b02218

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Density Functional Theory Calculations of Oxygen Vacancy Formation and Subsequent Molecular Adsorption on Oxide Surfaces2018

    • Author(s)
      Hinuma Yoyo、Toyao Takashi、Kamachi Takashi、Maeno Zen、Takakusagi Satoru、Furukawa Shinya、Takigawa Ichigaku、Shimizu Ken-ichi
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 122 Issue: 51 Pages: 29435-29444

    • DOI

      10.1021/acs.jpcc.8b11279

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Premodified Surface Method to Obtain Ultra-highly Dispersed Metals and their 3D Structure Control on an Oxide Single-crystal Surface2018

    • Author(s)
      Takakusagi Satoru、Iwasawa Yasuhiro、Asakura Kiyotaka
    • Journal Title

      The Chemical Record

      Volume: 18 Issue: 7 Pages: 1-13

    • DOI

      10.1002/tcr.201800088

    • NAID

      120006866530

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Presentation] オペランド偏光全反射蛍光XAFS法の開発による動作中触媒表面の三次元構造解析2021

    • Author(s)
      高草木達
    • Organizer
      令和2年度日本表面真空学会東北・北海道支部学術講演会
    • Related Report
      2020 Annual Research Report
    • Invited
  • [Presentation] Operando PTRF-XAFS study of 3D structure determination of active metal species on a model catalyst surface under working conditions2021

    • Author(s)
      BANG Lu、TAKAKUSAGI Satoru、KIDO Daiki、ASAKURA Kiyotaka
    • Organizer
      第34回日本放射光学会年会・放射光科学合同シンポジウム
    • Related Report
      2020 Annual Research Report
  • [Presentation] Atomic-level visualization of surface catalytic reactions by in-situ/operando XAFS and STM2020

    • Author(s)
      TAKAKUSAGI Satoru
    • Organizer
      International Joint Symposium On-Line: Cutting Edge of Surface Science For Atomic Scale Approach to Catalyst
    • Related Report
      2020 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 単結晶モデル表面を用いた触媒反応プロセスの原子レベル可視化2020

    • Author(s)
      高草木達
    • Organizer
      触媒学会北海道支部 札幌講演会
    • Related Report
      2020 Annual Research Report
    • Invited
  • [Presentation] Development of operando PTRF-XAFS technique for elucidating 3D structure-activity relationship in heterogeneous catalysis2020

    • Author(s)
      TAKAKUSAGI Satoru、BANG Lu、KIDO Daiki、SATO Yuta、ASAKURA Kiyotaka
    • Organizer
      The 2nd Workshop of Reaction Infography / The 3rd IRCCS International Symposium
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Development of operando PTRF-XAFS technique for elucidating 3D structure-activity relationship in heterogeneous catalysis2019

    • Author(s)
      TAKAKUSAGI Satoru、BANG Lu、KIDO Daiki、SATO Yuta、ASAKURA Kiyotaka
    • Organizer
      21st International Vacuum Congress
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 触媒動作中の活性点三次元構造決定を可能とする オペランド偏光全反射蛍光XAFS法の開発2019

    • Author(s)
      高草木達、魯邦 、城戸大貴 、佐藤優太 、朝倉清高
    • Organizer
      第124回触媒討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Operando PTRF-XAFS technique for 3D structure determination of active metal sites on a model catalyst surface under working conditions2019

    • Author(s)
      TAKAKUSAGI Satoru、BANG Lu、KIDO Daiki、SATO Yuta、ASAKURA Kiyotaka
    • Organizer
      AVS 66th International Symposium & Exhibition 2019
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Development of operando PTRF-XAFS technique for determining 3D structure of active sites in heterogeneous catalysis2019

    • Author(s)
      TAKAKUSAGI Satoru
    • Organizer
      The 81st Okazaki Conference “Forefront of Measurement Technologies for Surface Chemistry and Physics in Real-Space, k-Space, and Real-Time”
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 触媒動作中の活性点三次元構造決定のためのオペランド 偏光全反射蛍光XAFS法の開発2019

    • Author(s)
      高草木達、魯邦 、城戸大貴 、佐藤優太 、朝倉清高
    • Organizer
      PF研究会「XAFS・X線顕微鏡分光分析分野でのIMSS,PF戦略的利用に関する研究会」
    • Related Report
      2019 Annual Research Report
    • Invited
  • [Presentation] 触媒動作中の活性点立体構造決定のためのオペランド偏光全反射蛍光XAFS法の開発と触媒インフォマティクス2019

    • Author(s)
      高草木達
    • Organizer
      第17回SPring-8ユーザー協同体顕微ナノ材料科学研究会・第14回日本表面科学会放射光表面科学研究部会・第3回プローブ顕微鏡研究部会合同シンポジウム
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] Atomic-level structure and reactivity on well-defined model catalysts surfaces studied by STM and XAFS2018

    • Author(s)
      TAKAKUSAGI Satoru、ASAKURA Kiyotaka
    • Organizer
      International Symposium on Advancement and Prospect of Catalysis Science & Technology
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 担持金属モデル触媒表面の原子レベル構造解析と反応計測2018

    • Author(s)
      高草木達
    • Organizer
      第122回触媒討論会
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] PTRF-XAFS法による酸化物上金属ナノ構造の三次元可視化と触媒インフォマティクスへの挑戦2018

    • Author(s)
      高草木達
    • Organizer
      PF研究会「量子ビームと新規合成手法の融合による酸化物の新機能探索」
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] PTRF-XAFS study of single metal dispersion on an oxide single crystal surface by premodification with a functional organic molecule2018

    • Author(s)
      TAKAKUSAGI Satoru、ASAKURA Kiyotaka
    • Organizer
      AVS 65th International Symposium & Exhibition
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 偏光全反射蛍光XAFS法を用いた固気及び固液界面における表面金属ナノ構造の三次元構造解析2018

    • Author(s)
      高草木達
    • Organizer
      2018年日本表面真空学会学術講演会
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Remarks] 北海道大学触媒科学研究所 規整表面ナノ構造研究クラスター <展開型>

    • Related Report
      2020 Annual Research Report
  • [Remarks] 北海道大学触媒科学研究所 規整表面ナノ構造研究クラスター <展開型>

    • URL

      http://www.cat.hokudai.ac.jp/kouzouseigyo.html

    • Related Report
      2019 Annual Research Report
  • [Remarks] 北海道大学触媒科学研究所触媒表面研究部門

    • URL

      http://www.cat.hokudai.ac.jp/asakura/

    • Related Report
      2018 Annual Research Report

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Published: 2018-04-23   Modified: 2022-01-27  

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