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Observation and control of transition state for catalytic reactions by using X-ray absorption spectroscopy

Research Project

Project/Area Number 17KT0007
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeMulti-year Fund
Section特設分野
Research Field Transition State Control
Research InstitutionKyoto University

Principal Investigator

Tanaka Tsunehiro  京都大学, 工学研究科, 教授 (70201621)

Project Period (FY) 2017-07-18 – 2020-03-31
Project Status Completed (Fiscal Year 2019)
Budget Amount *help
¥18,720,000 (Direct Cost: ¥14,400,000、Indirect Cost: ¥4,320,000)
Fiscal Year 2019: ¥2,990,000 (Direct Cost: ¥2,300,000、Indirect Cost: ¥690,000)
Fiscal Year 2018: ¥8,580,000 (Direct Cost: ¥6,600,000、Indirect Cost: ¥1,980,000)
Fiscal Year 2017: ¥7,150,000 (Direct Cost: ¥5,500,000、Indirect Cost: ¥1,650,000)
KeywordsX線吸収分光 / 赤外吸収分光 / オペランド分光 / CO2の水素化 / X線吸収分光法 / Operando測定 / SPring-8 / DRIFT-IR / その場観察 / 同時観察 / 自動車排ガス浄化触媒 / 触媒反応 / 構造変化速度論解析
Outline of Final Research Achievements

We elucidated the active sites for unfavorable CH4 formation over Al2O3-supported Pt catalyst during hydrogenation of CO2 at ambient pressure, by using a combination of X-ray absorption spectroscopy (XAS) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) with product analysis (operando XAS-DRIFTS). Bicarbonate species are formed on the Al2O3 surface upon adsorption of CO2 at the surface hydroxyl groups of Al2O3. Those bicarbonate species are hydrogenated toward CO by hydrogen spillover from Pt surface as the dissociation sites of H2. The combined data of XAS and DRIFTS revealed that CO species co-adsorbed with H on the perimeter Pt sites at the interface between Pt particles and Al2O3 surface, and then further hydrogenation of those CO species led to the CH4 formation.

Academic Significance and Societal Importance of the Research Achievements

不均一系触媒反応における反応機構を「基質や生成物などの分子の振る舞い」に加えて「触媒自体の構造変化」から速度論的に解釈するため,兵庫県佐用市光都に位置する大型放射光施設SPring-8内のBL01B1にX線吸収スペクトルと赤外吸収スペクトルを同時に測定しながら,触媒反応を観察することができるシステムを構築した.このシステムを用いてAl2O3担持Pt触媒上でのCO2の水素化の反応機構解析を行い,詳細な反応メカニズムを提案した.

Report

(4 results)
  • 2019 Annual Research Report   Final Research Report ( PDF )
  • 2018 Research-status Report
  • 2017 Research-status Report
  • Research Products

    (18 results)

All 2020 2019 2018 2017

All Journal Article (5 results) (of which Peer Reviewed: 3 results) Presentation (13 results) (of which Int'l Joint Research: 3 results,  Invited: 2 results)

  • [Journal Article] Isolated Platinum Atoms in Ni/γ-Al2O3 for Selective Hydrogenation of CO2 toward CH42019

    • Author(s)
      Kikkawa Soichi、Teramura Kentaro、Asakura Hiroyuki、Hosokawa Saburo、Tanaka Tsunehiro
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 123 Issue: 38 Pages: 23446-23454

    • DOI

      10.1021/acs.jpcc.9b03432

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Self-regeneration of a Ni-Cu alloy catalyst during a three-way catalytic reaction2019

    • Author(s)
      H. Asakura, T. Onuki, S. Hosokawa, N. Takagi, S. Sakaki, K. Teramura, and T. Tanaka
    • Journal Title

      Phys. Chem. Chem. Phys.

      Volume: 21 Issue: 35 Pages: 18816-18822

    • DOI

      10.1039/c9cp01884k

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] A feasibility study of “range-extended” EXAFS measurement at the Pt L3-edge of Pt/Al2O3 in the presence of Au2O32018

    • Author(s)
      Asakura Hiroyuki、Kawamura Naomi、Mizumaki Masaichiro、Nitta Kiyofumi、Ishii Kenji、Hosokawa Saburo、Teramura Kentaro、Tanaka Tsunehiro
    • Journal Title

      Journal of Analytical Atomic Spectrometry

      Volume: 33 Issue: 1 Pages: 84-89

    • DOI

      10.1039/c7ja00309a

    • Related Report
      2017 Research-status Report
  • [Journal Article] Oxygen Storage Property and Chemical Stability of SrFe1?xTixO3?δ with Robust Perovskite Structure2017

    • Author(s)
      Demizu Akito、Beppu Kosuke、Hosokawa Saburo、Kato Kazuo、Asakura Hiroyuki、Teramura Kentaro、Tanaka Tsunehiro
    • Journal Title

      J. Phys. Chem. C

      Volume: 121 Issue: 35 Pages: 19358-19364

    • DOI

      10.1021/acs.jpcc.7b06078

    • Related Report
      2017 Research-status Report
  • [Journal Article] Dynamic Behavior of Rh Species in Rh/Al2O3 Model Catalyst during Three-Way Catalytic Reaction: An Operando X-ray Absorption Spectroscopy Study2017

    • Author(s)
      Asakura Hiroyuki、Hosokawa Saburo、Ina Toshiaki、Kato Kazuo、Nitta Kiyofumi、Uera Kei、Uruga Tomoya、Miura Hiroki、Shishido Tetsuya、Ohyama Junya、Satsuma Atsushi、Sato Katsutoshi、Yamamoto Akira、Hinokuma Satoshi、Yoshida Hiroshi、Machida Masato、Yamazoe Seiji、Tsukuda Tatsuya、Teramura Kentaro、Tanaka Tsunehiro
    • Journal Title

      Journal of the American Chemical Society

      Volume: 140 Issue: 1 Pages: 176-184

    • DOI

      10.1021/jacs.7b07114

    • NAID

      120006394775

    • Related Report
      2017 Research-status Report
    • Peer Reviewed
  • [Presentation] Niに配位された孤立Pt種上での高選択的なCO2メタン化2020

    • Author(s)
      吉川聡一,寺村謙太郎,朝倉博行,細川三郎,田中庸裕
    • Organizer
      第125回触媒討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] CO2の水素化に有効なFe系酸化物前駆体の検討2020

    • Author(s)
      松尾紘希・吉川聡一・寺村謙太郎・細川三郎・朝倉博行・田中庸裕
    • Organizer
      日本化学会第100春季年会
    • Related Report
      2019 Annual Research Report
  • [Presentation] CO2の水素化に異なる生成物選択性を示す担持Pt触媒のOperando XAS-DRIFTS計測2019

    • Author(s)
      吉川聡一,寺村謙太郎, 朝倉博行, 細川三郎, 田中庸裕
    • Organizer
      第124回触媒討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Enhancement of CO evolution by Yb modification technique of Ga2O3 for the photocatalytic conversion of CO2 by H2O2019

    • Author(s)
      KIKKAWA Soichi; TERAMURA Kentaro; ASAKURA Hiroyuki; HOSOKAWA Saburo; TANAKA Tsunehiro
    • Organizer
      The 17th Korea-Japan Symposium on Catalysis
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] High catalytic activity of isolated Pt atoms of Ni-Pt alloy for CO2 hydrogenation2018

    • Author(s)
      Soichi KIKKAWA, Kentaro TERAMURA, Hiroyuki ASAKURA, Saburo HOSOKAWA, Tsunehiro TANAKA
    • Organizer
      The 8th Tokyo Conference on Advanced Catalytic Science and Technology (TOCAT8)
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] In-situ XAFS を用いた担持 Pt ナノ粒子の還元機構の解明2018

    • Author(s)
      吉川聡一,寺村謙太郎, 朝倉博行, 細川三郎, 田中庸裕
    • Organizer
      第21回 XAFS討論会
    • Related Report
      2018 Research-status Report
  • [Presentation] Niに囲まれた孤立Pt種上でのCO2の水素化2018

    • Author(s)
      吉川聡一,寺村謙太郎, 朝倉博行, 細川三郎, 田中庸裕
    • Organizer
      第122回触媒討論会
    • Related Report
      2018 Research-status Report
  • [Presentation] CO2 hydrogenation over isolated Pt atoms of Ni-Pt alloy2018

    • Author(s)
      Soichi KIKKAWA, Kentaro TERAMURA, Hiroyuki ASAKURA, Saburo HOSOKAWA, Tsunehiro TANAKA
    • Organizer
      Osaka-kansai International Symposium on Catalysis
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] CO2 hydrogenation over isolated Pt atoms surrounded by Ni atoms in Ni-Pt alloy catalyst2018

    • Author(s)
      KIKKAWA, Soichi; TERAMURA, Kentaro; ASAKURA, Hiroyuki; HOSOKAWA, Saburo; TANAKA, Tsunehiro
    • Organizer
      日本化学会第99春季年会
    • Related Report
      2018 Research-status Report
  • [Presentation] 貴金属使用量減量を指向した自動車排ガス浄化触媒2017

    • Author(s)
      田中庸裕
    • Organizer
      第28回グリーンケミストリーフォーラム
    • Related Report
      2017 Research-status Report
    • Invited
  • [Presentation] Cu-Ni合金触媒を用いた三元触媒反応に対する酸素濃度依存性2017

    • Author(s)
      小貫哲雄,朝倉博行,細川三郎,寺村謙太郎,田中庸裕
    • Organizer
      第120回触媒討論会
    • Related Report
      2017 Research-status Report
  • [Presentation] Operando XAFS による三元触媒反応中の Rh/Al2O3 モデル触媒における Rh 種の動的挙動2017

    • Author(s)
      朝倉博行,細川三郎,寺村謙太郎,田中庸裕
    • Organizer
      第120回触媒討論会
    • Related Report
      2017 Research-status Report
  • [Presentation] 貴金属使用量減量を指向した自動車排ガス浄化触媒2017

    • Author(s)
      田中庸裕
    • Organizer
      「自動車排気触媒システムの多様性への対応」シンポジウム
    • Related Report
      2017 Research-status Report
    • Invited

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Published: 2017-07-21   Modified: 2021-02-19  

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