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Atomic-level understanding of catalytic reaction processes by operando observation of 3D active structures and surface-adsorbed species

Research Project

Project/Area Number 21H01802
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, 教授 (30359484)

Project Period (FY) 2021-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥18,330,000 (Direct Cost: ¥14,100,000、Indirect Cost: ¥4,230,000)
Fiscal Year 2023: ¥780,000 (Direct Cost: ¥600,000、Indirect Cost: ¥180,000)
Fiscal Year 2022: ¥780,000 (Direct Cost: ¥600,000、Indirect Cost: ¥180,000)
Fiscal Year 2021: ¥16,770,000 (Direct Cost: ¥12,900,000、Indirect Cost: ¥3,870,000)
Keywordsオペランド偏光全反射蛍光XAFS法 / オペランド偏光変調赤外反射分光法 / 活性点三次元構造解析 / 担持金属触媒 / 複合表面計測 / 表面吸着種解析 / 反応機構解明 / 単結晶モデル触媒表面 / 偏光全反射蛍光XAFS法 / 偏光変調赤外反射分光法 / オペランド計測 / 担体効果
Outline of Research at the Start

固体触媒において、「触媒反応中にどういった電子状態及び立体構造(三次元原子配列)を有する活性ナノ構造が形成され、そこには吸着種がどのような状態で存在して最終生成物を与えるのか?」を解明することは、表面ナノ構造と触媒活性との相関および反応機構を真に理解し、更なる高活性化への指針を得るために不可欠である。本研究では、超高真空~大気圧下で触媒動作中活性点の電子状態及び立体構造が得られるオペランド偏光全反射蛍光XAFS法に加え、新たにオペランド偏光変調赤外反射分光法を開発し、吸着種挙動解析も可能とする複合オペランド表面計測システムを確立する。さらに酸化物担持金属触媒における担体効果の解明を試みる。

Outline of Final Research Achievements

Oxide-supported metal catalysts, in which active metal species (monatomic or nanoparticles) are supported on oxide surfaces, are the most widely used in practical applications. In order to understand catalytic reaction processes and to provide guidelines for further improvement of catalytic performance, it is essential to clarify factors affecting catalytic performance (electronic state and 3D structure of active metal sites and behavior of surface adsorbed species) under reaction conditions, and then to obtain information on precise structure-activity relationships and reaction mechanisms. In this study, the operando polarization-dependent total reflection fluorescence XAFS (PTRF-XAFS) technique developed in the 18H01864 project was upgraded and improved, and a new operando-polarized-modulation infrared reflection absorption spectroscopy was developed to evaluate all the factors affecting catalytic performance.

Academic Significance and Societal Importance of the Research Achievements

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おり、SDG実現に向けて触媒の更なる高性能化(極めて高い効率で欲しい物質だけを得る)が求められている。しかし、「触媒反応中にどういった電子状態及び立体構造を有する表面ナノ構造が形成され、そこには吸着種がどのような状態で存在して最終生成物を与えるのか?」という触媒制御因子に関する情報を得る評価技術は確立されておらず、厳密な構造-活性相関の取得や反応機構の解明は難しかった。本研究によって、こうした情報の取得が可能になり、今後の触媒設計に関してより明確な指針を与えることが期待できる。

Report

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

    (40 results)

All 2024 2023 2022 2021 Other

All Journal Article (11 results) (of which Int'l Joint Research: 2 results,  Peer Reviewed: 11 results,  Open Access: 4 results) Presentation (26 results) (of which Int'l Joint Research: 16 results,  Invited: 15 results) Remarks (3 results)

  • [Journal Article] <i>In situ</i> Study on Structure of a Diluted Pt/HOPG Model Catalyst System Prepared by the Two-phase Liquid Reduction Method Using a Novel BCLA/HERFD+BI-XAFS Method2024

    • Author(s)
      Dong Kaiyue、Hu Bing、Rashid Md Harun Al、Lu Bang、Miyabayashi Keiko、Higashi Kotaro、Uruga Tomoya、Iwasawa Yasuhiro、Kido Daiki、Takakusagi Satoru、Asakura Kiyotaka
    • Journal Title

      e-Journal of Surface Science and Nanotechnology

      Volume: 22 Issue: 2 Pages: 129-137

    • DOI

      10.1380/ejssnt.2024-004

    • ISSN
      1348-0391
    • Year and Date
      2024-02-15
    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Dynamic Behavior of Intermediate Adsorbates to Control Activity and Product Selectivity in Heterogeneous Catalysis: Methanol Decomposition on Pt/TiO2(110)2023

    • Author(s)
      Liu Can、Lu Bang、Ariga-Miwa Hiroko、Ogura Shohei、Ozawa Takahiro、Fukutani Katsuyuki、Gao Min、Hasegawa Jun-ya、Shimizu Ken-ichi、Asakura Kiyotaka、Takakusagi Satoru
    • Journal Title

      Journal of the American Chemical Society

      Volume: 145 Issue: 36 Pages: 19953-19960

    • DOI

      10.1021/jacs.3c06405

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Can amine ligands atomically disperse Cu atoms on TiO2(110)? Cu deposition on TiO2(110) premodified with o-anthranilic acid2023

    • Author(s)
      Kim Cho Rong、Maeda Honoka、Lu Bang、Nakamura Yuto、Lin Yunli、Wakisaka Yuki、Kido Daiki、Asakura Kiyotaka、Takakusagi Satoru
    • Journal Title

      Chemistry Letters

      Volume: 53 Issue: 2

    • DOI

      10.1093/chemle/upad045

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] The Effect of Structural Change during the Activation Process on the Catalysis of In/SiO2 Nonoxidative Coupling of Methane: An Operando XAFS Study2023

    • Author(s)
      Wada Takahiro、Kashaboina Upendar、Nishikawa Yuta、Wakisaka Yuki、Bao Deling、Takakusagi Satoru、Inami Yuta、Kuriyama Fumiya、Dipu Arnoldus Lambertus、Ogihara Hitoshi、Iguchi Shoji、Yamanaka Ichiro、Kido Daiki、Kimura Masao、Uo Motohiro、Asakura Kiyotaka
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 127 Issue: 50 Pages: 24211-24222

    • DOI

      10.1021/acs.jpcc.3c04539

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Stacking of a Cofacially Stacked Iron Phthalocyanine Dimer on Graphite Achieved High Catalytic CH<sub>4</sub> Oxidation Activity Comparable to That of pMMO2023

    • Author(s)
      Yamada Yasuyuki、Morita Kentaro、Sugiura Takuya、Toyoda Yuka、Mihara Nozomi、Nagasaka Masanari、Takaya Hikaru、Tanaka Kiyohisa、Koitaya Takanori、Nakatani Naoki、Ariga-Miwa Hiroko、Takakusagi Satoru、Hitomi Yutaka、Kudo Toshiji、Tsuji Yuta、Yoshizawa Kazunari、Tanaka Kentaro
    • Journal Title

      JACS Au

      Volume: 3 Issue: 3 Pages: 823-833

    • DOI

      10.1021/jacsau.2c00618

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Cooperative Catalysis of Vibrationally Excited CO2 and Alloy Catalyst Breaks the Thermodynamic Equilibrium Limitation2022

    • Author(s)
      Dae-Yeong Kim, Hyungwon Ham, Xiaozhong Chen, Shuai Liu, Haoran Xu, Bang Lu, Shinya Furukawa, Hyun-Ha Kim, Satoru Takakusagi, Koichi Sasaki, and Tomohiro Nozak
    • Journal Title

      J. Am. Chem. Soc.

      Volume: 144 Issue: 31 Pages: 14140-14149

    • DOI

      10.1021/jacs.2c03764

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] High-Entropy Intermetallics Serve Ultrastable Single-Atom Pt for Propane Dehydrogenation2022

    • Author(s)
      Nakaya Yuki、Hayashida Eigo、Asakura Hiroyuki、Takakusagi Satoru、Yasumura Shunsaku、Shimizu Ken-ichi、Furukawa Shinya
    • Journal Title

      Journal of the American Chemical Society

      Volume: 144 Issue: 35 Pages: 15944-15953

    • DOI

      10.1021/jacs.2c01200

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Metastable Structure of Photoexcited WO3 Determined by the Pump-probe Extended X-ray Absorption Fine Structure Spectroscopy and Constrained Thorough Search Analysis2022

    • Author(s)
      Kido Daiki、Uemura Yohei、Wakisaka Yuki、Koide Akihiro、Uehara Hiromitsu、Niwa Yasuhiro、Nozawa Shunsuke、Ichiyanagi Kohei、Fukaya Ryo、Adachi Shin-ichi、Sato Tokushi、Jenkins Harry、Yokoyama Toshihiko、Takakusagi Satoru、Hasegawa Jun-ya、Asakura Kiyotaka
    • Journal Title

      Chemistry Letters

      Volume: 51 Issue: 11 Pages: 1083-1086

    • DOI

      10.1246/cl.220381

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Abnormal Metal Bond Distances in PtAu Alloy Nanoparticles: In Situ Back-Illumination XAFS Investigations of the Structure of PtAu Nanoparticles on a Flat HOPG Substrate Prepared by Arc Plasma Deposition2022

    • Author(s)
      Hu Bing、Bharate Bapurao、Jimenez Juan D.、Lauterbach Jochen、Todoroki Naoto、Wadayama Toshimasa、Higashi Kotaro、Uruga Tomoya、Iwasawa Yasuhiro、Ariga-Miwa Hiroko、Takakusagi Satoru、Asakura Kiyotaka
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 126 Issue: 2 Pages: 1006-1016

    • DOI

      10.1021/acs.jpcc.1c08393

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Development of Operando Polarization-Dependent Total Reflection Fluorescence X-ray Absorption Fine Structure Technique for Three-Dimensional Structure Determination of Active Metal Species on a Model Catalyst Surface under Working Conditions2021

    • Author(s)
      Bang Lu, Daiki Kido, Yuta Sato, Haoran Xu, Wang-Jae Chun, Kiyotaka Asakura, Satoru Takakusagi,
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 125 Issue: 22 Pages: 12424-12432

    • DOI

      10.1021/acs.jpcc.1c02913

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Analysis of Updated Literature Data up to 2019 on the Oxidative Coupling of Methane Using an Extrapolative Machine‐Learning Method to Identify Novel Catalysts2021

    • Author(s)
      Mine Shinya、Takao Motoshi、Yamaguchi Taichi、Toyao Takashi、Maeno Zen、Hakim Siddiki S. M. A.、Takakusagi Satoru、Shimizu Ken‐ichi、Takigawa Ichigaku
    • Journal Title

      ChemCatChem

      Volume: 13 Issue: 16 Pages: 3636-3655

    • DOI

      10.1002/cctc.202100495

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Presentation] 放射光と表面科学を用いた触媒活性点の原子レベル構造解析2024

    • Author(s)
      高草木達
    • Organizer
      北海道大学触媒科学研究所・立命館大学SRセンター共催シンポジウム「触媒科学と放射光-Soft~Tender X線の新たな展開
    • Related Report
      2023 Annual Research Report
    • Invited
  • [Presentation] 不均一な構造を有する触媒材料における構造・活性相関の評価:単結晶モデル触媒を用いたアプローチ2024

    • Author(s)
      高草木達
    • Organizer
      2023年度量子ビームサイエンスフェスタ
    • Related Report
      2023 Annual Research Report
    • Invited
  • [Presentation] Operando PTRF-XAFS technique for elucidating relationship between 3D structure of active metal sites under working conditions2024

    • Author(s)
      Bang Lu, Daiki Kido, Haoran Xu, Kiyotaka Asakura, Satoru Takakusagi
    • Organizer
      International Symposium on Atomic Level Characterizations in Winter 2024 (ALC-W 2024)
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Diffusion and adsorbate-adsorbate interaction of methoxy intermediates adsorbed on Ti sites of a Pt/TiO2(110) surface2024

    • Author(s)
      Can Liu, Bang Lu, Hiroko Ariga Miwa, Min Gao, Jun-ya Hasegawa, Ken-ichi Shimizu, Kiyotaka Asakura, Satoru Takakusagi
    • Organizer
      International Symposium on Frontier of Nano- & Atomic-Scale Characterization 2023 (NanospecFY2023)
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] その場/オペランド表面科学計測による触媒反応の原子レベル可視化2023

    • Author(s)
      高草木達
    • Organizer
      第452回触媒科学研究所コロキウム
    • Related Report
      2023 Annual Research Report
    • Invited
  • [Presentation] Atomic-level visualization of surface catalytic reactions by in situ/operando surface science techniques2023

    • Author(s)
      Satoru Takakusagi
    • Organizer
      ICAT-FHI Symposium: Approaching to the Catalysis Reality
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 不均一な構造を有する固体触媒の放射光を用いた構造解析:不均一性への挑戦2023

    • Author(s)
      高草木達
    • Organizer
      第132回触媒討論会
    • Related Report
      2023 Annual Research Report
    • Invited
  • [Presentation] Dynamic Behavior of Intermediate Adsorbates to Control Activity and Product Selectivity in Heterogeneous Catalysis: Methanol Decomposition on Pt/TiO2(110)2023

    • Author(s)
      Satoru Takakusagi
    • Organizer
      MIRAI 2.0 Research and Innovation Week 2023 Materials Science TEG 2023
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Development of synchrotron X-ray and surface science techniques for characterizing plasma catalysis2023

    • Author(s)
      Satoru Takakusagi
    • Organizer
      2023 Australia-Japan Symposium on Plasma Catalysis
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Plasma-assisted nitrogen fixation and ammonia synthesis on Co surface at room temperature2023

    • Author(s)
      Bang Lu, Haoran Xu, Kiyotaka Asakura, Satoru Takakusagi
    • Organizer
      2023 Australia-Japan Symposium on Plasma Catalysis
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] オペランド偏光全反射蛍光XAFS法による触媒動作中の活性点三次元構造解析2023

    • Author(s)
      高草木達
    • Organizer
      第12 回 岩澤コンファレンス「 サステナブル社会のための触媒化学・表面科学の最前線 」
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] 圧力ギャップフリー触媒表面科学を目指して:現状と課題2023

    • Author(s)
      高草木達
    • Organizer
      触媒科学計測共同研究拠点ミニシンポジウム「超高速データ駆動科学と先端計測技術の融合による触媒科学イノベーション」
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] Development of operando PTRF-XAFS technique for precise 3D structure determination of active metal sites in heterogeneous catalysis2022

    • Author(s)
      Satoru Takakusagi
    • Organizer
      International Symposium on Next Generation Synchrotron Radiation Facility Utilization for Catalysts Characterization as Post Symposium of TOCAT
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Operando PTRF-XAFS technique for precise 3D structure determination of active metal sites in heterogeneous catalysis2022

    • Author(s)
      Satoru Takakusagi
    • Organizer
      ICAT-FHI Symposium: New Dimension of Catalytic Surface Study
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Elucidation of Precise 3D Structure-Activity Relationship in Heterogeneous Catalysis by Operando PTRF-XAFS Technique2022

    • Author(s)
      Unraveling 3D structure of active metal sites on catalyst surfaces under working conditions by operando PTRF-XAFS technique
    • Organizer
      IMS-ICAT Joint Symposium: Surface Science for Catalysis
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Unraveling 3D structure of active metal sites on catalyst surfaces under working conditions by operando PTRF-XAFS technique2022

    • Author(s)
      Unraveling 3D structure of active metal sites on catalyst surfaces under working conditions by operando PTRF-XAFS technique
    • Organizer
      MIRAI 2.0 Research and Innovation Week 2022 Materials Science TEG 2022
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 偏光XAFSと単結晶モデル表面を用いた触媒活性点のオペランド三次元構造解析2022

    • Author(s)
      高草木達
    • Organizer
      触媒学会界面分子変換研究会ワークショップ『固体触媒の活性構造を知る』
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] Elucidating the relationship between 3D structure and CO oxidation activity of Pt clusters on α-Al2O3(0001) using operando PTRF-XAFS2022

    • Author(s)
      B. Lu, D. Kido, H. Xu, K. Asakura, S. Takakusagi
    • Organizer
      The 22nd International Vacuum Congress (IVC-22)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Dynamic Behaviors of Intermediate Adsorbates Controlling Activity and Product Selectivity in Heterogeneous Catalysis: Methanol Decomposition on Pt/TiO2(110)2022

    • Author(s)
      C. Liu, H. Ariga-Miwa, S. Ogura, K. Fukutani, M. Gao, J. Hasegawa, K. Shimizu, K. Asakura, S.Takakusagi
    • Organizer
      The 22nd International Vacuum Congress (IVC-22)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 3D structure of atomically dispersed Cu on the TiO2(110) surface premodified with a nitrogen-containing compound2022

    • Author(s)
      C.R. Kim, B. Lu, Y. Nakamura, Y. Wakisaka, S. Takakusagi, K. Asakura
    • Organizer
      The 22nd International Vacuum Congress (IVC-22)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 含窒素カルボン酸化合物で前修飾された TiO2(110)表面上の Cu 原 子分散の構造解析2022

    • Author(s)
      金 チョロン、魯 邦、中村 優斗、脇坂 祐輝、高草木 達、朝倉 清高
    • Organizer
      日本化学会 第102春季年会 (2022)
    • Related Report
      2021 Annual Research Report
  • [Presentation] オペランド偏光全反射蛍光XAFS法の開発による 触媒反応中金属活性点の三次元構造解析2021

    • Author(s)
      高草木達、魯邦、城戸大貴、徐浩然、田旺帝、朝倉清高
    • Organizer
      第24回XAFS討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] Operando PTRF-XAFS technique for elucidating relationship between 3D structure of active metal sites and catalytic properties under working conditions2021

    • Author(s)
      TAKAKUSAGI Satoru、BANG Lu、XU Haoran、KIDO Daiki、ASAKURA Kiyotaka
    • Organizer
      The 2021 International Chemical Congress of Pacific Basin Societies (Pacifichem2021))
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 3D structure determination of active Pt clusters on an α-Al2O3(0001) surface during CO oxidation by operando PTRF-XAFS technique2021

    • Author(s)
      BANG Lu、TAKAKUSAGI Satoru、KIDO Daiki、SATO Yuta、XU Haoran、ASAKURA Kiyotaka
    • Organizer
      18th International Conference on X-ray Absorption Fine Structure (XAFS2021)
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Operando PTRF-XAFS study of 3D structure determination of active Pt species on an Al2O3 single-crystal surface during CO oxidation2021

    • Author(s)
      BANG Lu、TAKAKUSAGI Satoru、KIDO Daiki、XU Haoran、ASAKURA Kiyotaka
    • Organizer
      The 2021 International Chemical Congress of Pacific Basin Societies (Pacifichem2021))
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Monitoring 3D structure of active Pt clusters on α-Al2O3(0001) during CO oxidation using operando PTRF-XAFS technique2021

    • Author(s)
      BANG Lu、TAKAKUSAGI Satoru、KIDO Daiki、XU Haoran、ASAKURA Kiyotaka
    • Organizer
      第128回触媒討論会
    • Related Report
      2021 Annual Research Report
  • [Remarks] 北海道大学触媒科学研究所触媒構造研究部門

    • URL

      https://www.cat.hokudai.ac.jp/takakusagi/

    • Related Report
      2023 Annual Research Report
  • [Remarks] 北海道大学触媒科学研究所触媒構造研究部門

    • URL

      https://www.cat.hokudai.ac.jp/CatalystStructureResearchDivision.html

    • Related Report
      2022 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

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

    • Related Report
      2021 Annual Research Report

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Published: 2021-04-28   Modified: 2025-01-30  

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