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Structure dynamics at catalyst surfaces

Research Project

Project/Area Number 16072204
Research Category

Grant-in-Aid for Scientific Research on Priority Areas

Allocation TypeSingle-year Grants
Review Section Science and Engineering
Research InstitutionThe University of Tokyo

Principal Investigator

IWASAWA Yasuhiro  The University of Tokyo, Department of Chemistry, Professor (40018015)

Co-Investigator(Kenkyū-buntansha) MU Xindong  The University of Tokyo, Department of Chemistry, Assinstant Professor (20422363)
NOMURA Masaharu  High Energy Accelerator Research Organization, Institute of Materials Structure Science Photon Factory, Professor (70156230)
佐々木 岳彦  東京大学, 大学院・新領域創成科学研究科, 助教授 (90242099)
Project Period (FY) 2004 – 2006
Project Status Completed (Fiscal Year 2006)
Budget Amount *help
¥104,700,000 (Direct Cost: ¥104,700,000)
Fiscal Year 2006: ¥29,000,000 (Direct Cost: ¥29,000,000)
Fiscal Year 2005: ¥47,400,000 (Direct Cost: ¥47,400,000)
Fiscal Year 2004: ¥28,300,000 (Direct Cost: ¥28,300,000)
KeywordsCatalyst surface / X-ray a bsorption fine structure(XAFS) / Time-resolved XAFS / Scanning tunneling microscope(STM) / Direct phenol synthesis / Photo-oxidation catalysis / Catalytic reaction meachanism / In situ characterization / X線吸収微細構造 / 選択酸化 / In-situ解析 / 触媒 / 表面 / 分子構造 / ダイナミクス / 触媒作用 / SPM / XAFS / 時間分解構造解析 / DXAFS / 可視光反応 / TiO2 / セリア-ジルコニア固溶体 / ヒドロホルミル化 / 光触媒
Research Abstract

We studied the catalytically active structure, its structural transformation and dynamics, and reaction mechanism for direct phenol synthesis from benzene and molecular oxygen on a novel N-interstitial Re_<10>-cluster catalyst supported on HZSM-5 zeolite, which exhibited remarkable performances for the direct phenol synthesis. The active N-interstitial Re_<10> cluster was produced by NH_3 and it was the active species for the direct phenol synthesis using O_2 as an oxidant. Molecular oxygen (O_2) was suggested to directly react with benzene without dissociation to atomic oxygen (Ea (activation energy) = 24 kJ mol^<-1>) and the active Re cluster dynamically converted to inactive Re monomers under the reaction conditions. The structural transformation between the Re cluster and the Re monomers cycled during the phenol synthesis, whose mechanism was studied by in-situ time-resolved XAFS techniques.
TiO_2 is a typical functional metal oxide which exhibits photocatalysis. Usually only ultraviolet light must be used for photochemical reactions on TiO_2 because of its bulk band gap. However, we discovered visible light photo-oxidation reactions of formic acid on the ordered lattice-work structure of a TiO_2(001) surface by using scanning tunneling microscopy (STM). Two photon photoelectron and electron energy loss spectroscopies and density functional theory calculations revealed that the nanostructured surface makes the band gap significantly smaller than 3.0 eV only at the surface layer and that the surface state of the crystal enables visible light response.

Report

(4 results)
  • 2006 Annual Research Report   Final Research Report Summary
  • 2005 Annual Research Report
  • 2004 Annual Research Report
  • Research Products

    (45 results)

All 2007 2006 2005 2004 Other

All Journal Article (33 results) (of which Peer Reviewed: 3 results) Presentation (8 results) Book (3 results) Remarks (1 results)

  • [Journal Article] Density Functional Theoretical Calculations for a Co_2/γ-Al_2O_3 Model Catalyst : Structures of the γ-Al_2O_3 Bulk and Surface and Attachment Sites for Co^<2+> Ions2006

    • Author(s)
      T. Taniike, M. Tada, Y. Morikawa, T. Sasaki, Y. Iwasawa
    • Journal Title

      J. Phys. Chem. B 110

      Pages: 4929-4936

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] Ni Ion-Containing Ionic Liquid Salt and Ni Ion-Containing Immobilized Ionic Liquid on Silica : Application to Suzuki Cross-Coupling Reactions Between Chloroarenes and Arylboronic Acids2006

    • Author(s)
      C. Zhong, T. Sasaki, M. Tada, Y. Iwasawa
    • Journal Title

      J. Catal. 242

      Pages: 357-364

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] Advanced Chemical Design with Supported Metal Complexes for Selective Catalysis2006

    • Author(s)
      M. Tada, Y. Iwasawa
    • Journal Title

      Chem. Commun.

      Pages: 2833-2844

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] Density Functional Theoretical Calculations for a Co_2/ γ -Al_2O_3 Model Catalyst : Structures of the γ -Al_2O_3 Bulk and Surface and Attachment Sites for Co^<2+> Ions2006

    • Author(s)
      T. Taniike, M. Tada, Y. Morikawa, T. Sasaki, Y. Iwasawa
    • Journal Title

      J. Phys. Chem. B 110

      Pages: 4929-4936

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Structure and Reaction Control at Catalyst Surfaces2006

    • Author(s)
      M. Tada, Y. Iwasawa
    • Journal Title

      Surface and Nanomolecular Catalysis Taylor & Francis

      Pages: 229-256

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Density Functional Theoretical Calculations for a Co_2/γ-Al_2O_3 Model Catalyst : Structures of γ-Al_2O_3 Bulk and Surface and Attachment Sites for Co^<2+> Ions2006

    • Author(s)
      T.Taniike, M.Tada, Y.Morikawa, T.Sasaki, Y.Iwasawa
    • Journal Title

      J. Phys. Chem. B 110

      Pages: 4929-4936

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Advanced Catalyst Design with Supported Metal Complexes for Selective Catalysis2006

    • Author(s)
      M.Tada, Y.Iwasawa
    • Journal Title

      Chem. Commun.

      Pages: 2833-2844

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Surface-Promoted Reductive Synthesis of Supported Metallic Cu Nanoparticles Active for Selective Dehydrogenation of Methanol2006

    • Author(s)
      M.Tada, R.Bal, S.Namba, Y.Iwasawa
    • Journal Title

      Appl. Catal. A : General 307

      Pages: 78-84

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Ni Ion-Containing Ionic Liquid Salt and Ni Ion-Containing Immobilized Ionic Liquid on Silica : Application to Suzuki Cross Coupling Reactions between Chloroarenes and Arylboronic Acids2006

    • Author(s)
      C.Zhong, T.Sasaki, M.Tada, Y.Iwasawa
    • Journal Title

      J. Catal. 242

      Pages: 357-364

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Direct Phenol Synthesis by Selective Oxidation of Benzene with Molecular Oxygen on an Interstitial-N/Re Cluster/Zeolite Catalyst2006

    • Author(s)
      R.Bal, M., Tada, T.Sasaki, Y.Iwasawa
    • Journal Title

      Angew.Chem.Int.Ed. 45

      Pages: 448-452

    • Related Report
      2005 Annual Research Report
  • [Journal Article] The Role of Carbon Dioxide in Chemoselective Hydrogenation of Halonitroaromatics over Supported Noble Metal Catalysts in Supercritical Carbon Dioxide2005

    • Author(s)
      S.Ichikawa, M.Tada, Y.Iwasawa, T.Ikariya
    • Journal Title

      Chem.Common.

      Pages: 924-925

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Bound Site of Mo Atoms and Its Local Structure in a Mo/HY Catalyst Characterized by Extended X-ray Absorption Fine Structure and Density Functional Calculation2005

    • Author(s)
      T.Sasaki, F.Nakagawa, Y.Iwasawa
    • Journal Title

      J.Phys.Chem.B 109

      Pages: 2128-2138

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Catalytic-Dehydrogenation of AliPhatic Amines to Nitriles, Imines, or Vinylamines and Dealkylation of Tertiary Aliphatic Amines over Halide Cluster Catalysts of Group 5 and 6 Transition Metals2005

    • Author(s)
      S.kamiguchi, A, Nakamura, A Suzuki, M Kodomari, M.Nomura Y.Iwasawa, T.Chihara
    • Journal Title

      J.Catal. 230

      Pages: 204-213

    • Related Report
      2005 Annual Research Report
  • [Journal Article] XAFS Study on the Local Structure of Zirconium Containing MesoPorous Silicas, Zr-MCM-41 and Their Catalytic Properties2005

    • Author(s)
      A.Yamaguchi, M.Yokoyama, A.Suzuki, Y.Iwasawa, H.Sakai, M.Yuasa, M.Abe
    • Journal Title

      Physica Scripta T115

      Pages: 834-836

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Time-Resolved Ehergy-Dispersive XAFS for In-stiu Chafacterization of Nano-Structures and Catalysts"2005

    • Author(s)
      Y.Iwasawa, A.Suzuki, M.Nomura
    • Journal Title

      Physica Scripta T115

      Pages: 59-65

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Chiral Self-Dimerization of Vanadium Complexes on a SiO2 Surface for Asymmetric Catalytic Coupling of 2-Naphthol : Structure, Performance,and Mechanism2005

    • Author(s)
      M.Tada, N.KoJima, Y.lzumi, T.Taniike, Y.Iwasawa
    • Journal Title

      J.Phys.Chem.B 109

      Pages: 9905-9916

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Immobilized Metal Ion-Containing Ionic Liquids : Preparation, Structure and Catalytic Performance in Kharasch Addition Reaction2005

    • Author(s)
      T.Sasaki, C.Zhong, M.Tada, Y.Iwasawa
    • Journal Title

      Chem.Commun.

      Pages: 2506-2508

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Surfactant-Promoted Novel Reductive Synthesis of Supported Metallic Cu Nanoclusters and Their Catalytic Performances for Selective Dehydrogenation of Methanol2005

    • Author(s)
      R.Bal, M.Tada, Y.Iwasawa
    • Journal Title

      Chem.Commun.

      Pages: 3433-3435

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Chemical Design and In Situ Characterization of Active Surfaces for Selective Catalysis2005

    • Author(s)
      M.Tada, Y.Iwasawa
    • Journal Title

      Annu. Rev.Mater.Res. 35

      Pages: 397-426

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Enantioselective Diels-Alder Reaction Promoted by Achiral Functionalization of a SiO2-supported Cu-BOX[BIS(oxazoline)]Catalyst2005

    • Author(s)
      M.Tada, S.Tanaka, Y.Iwasawa
    • Journal Title

      Chem.Lett. 34

      Pages: 1362-1363

    • NAID

      130004423698

    • Related Report
      2005 Annual Research Report
  • [Journal Article] X-ray Absorption Fine Structure Combined with X-ray Fluorescence Spectrometry. Part 15.Monitoring of Vanadium SiteTrans formations on Titania and in Mesoporous Titania by Selective Detection of the Vanadium k□1 Fluorescence2005

    • Author(s)
      Y.Izumi, F.Kiyotaki, N.Yagi, A.Vlaicu, A.Nisawa, S.Fukushima, H.Yoshitake, Y.Iwasawa
    • Journal Title

      J.Phys. Chem.B 109

      Pages: 14884-14891

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Structural Features of CeO2 (111)Revealed by Dynamic SFM2005

    • Author(s)
      S.Gritschneder, Y.Mamai, Y.Iwasawa, M.Reichling
    • Journal Title

      Nanotechnology 16

    • Related Report
      2005 Annual Research Report
  • [Journal Article] XAFS Characterization of Pt-Fe/Zeolite Catalysts for Preferential Oxidation of CO in Hydrogen Fuel Gases2005

    • Author(s)
      M.kotobuki, T.Shido, M.Tada, H.Uchida, H.Yamashita, Y.Iwasawa, M.Watanabe
    • Journal Title

      Catal.Lett. 103

      Pages: 263-269

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Oxygen Vacancy Promoting Catalytic Dehydration of Formic Acid on TiO2(110)by In Situ Scanning Tunneling Microscopic Observation2005

    • Author(s)
      M.Aizawa, Y.Morikawa, Y.Namai, H.Morikawa, Y.Iwasawa
    • Journal Title

      J.Phys.Chem.B 109

      Pages: 18831-18838

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Direct Phenol Synthesis from Benzene with Molecular Oxygen on Rhenium/Zeolite Catalysts2005

    • Author(s)
      R.Bal, M.Tada, T.Kusakari, Y.Iwasawa
    • Journal Title

      触媒 47

      Pages: 72-74

    • NAID

      10015432764

    • Related Report
      2005 Annual Research Report
  • [Journal Article] シリカ表面固定化不斉Cu-BOX錯体触媒の設計と不斉Diels-Alder反応-表面の有機官能基修飾による不斉誘起一2005

    • Author(s)
      田中里佳, 唯美津木, 岩澤康裕
    • Journal Title

      触媒 47

      Pages: 430-432

    • Related Report
      2005 Annual Research Report
  • [Journal Article] The Dynamic Behavior of CH_3OH and NO_2 Adsorbed on CeO_2(111) Studied by Noncontact Atomic Force Microscopy2004

    • Author(s)
      Y.Namai, K.Fukui, Y.Iwasawa
    • Journal Title

      Nanotechnology 15

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Design of a Novel Molecular-Imprinted Rh-Amine Complex on SiO_2 and Its Shape-Selective Catalysis for α-Methylstyrene Hydrogenation2004

    • Author(s)
      M.Tada, T.Sasaki, Y.Iwasawa
    • Journal Title

      Journal of Physical Chemistry B 108

      Pages: 2918-2918

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Selective Oxidation of Benzene to Phenol with Molecular Oxygen on Rhenium/Zeolite Catalysts2004

    • Author(s)
      T.Kusakari, T.Sasaki, Y.Iwasawa
    • Journal Title

      Chemical Communications

      Pages: 992-992

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Time-Scale and Sequence of Dynamic Structural changes in a MgO-Attached Ruthenium Cluster Catalyst Observed by In Situ Time-Resolved DXAFS2004

    • Author(s)
      A.Suzuki, A.Yamaguchi, T.Chihara, Y.Inada, M.Yuasa, M.Abe, M.Nomura.Y.Iwasawa
    • Journal Title

      Journal of Physical Chemistry B 108

      Pages: 5609-5609

    • Related Report
      2004 Annual Research Report
  • [Journal Article] First-Principles Theoretical Study and Scanning Tunneling Microscopic Observation of Dehydration Process of Formic Acid on a TiO2(110) Surface2004

    • Author(s)
      Y.Morikawa, I.Tkahashi, M.Airzawa, Y.Namai, T.Sasaki, Y.Iwasawa
    • Journal Title

      Journal of Physical Chemistry B 108

      Pages: 14446-14446

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Temporal Analysis of Products (TAP) Study on Low Temperature Carbon Monooxide Oxidation on Supported Au Catalysts

    • Author(s)
      M.Olea, M.Tada, Y.Iwasawa
    • Journal Title

      Topics Catal. (In press)

    • Related Report
      2006 Annual Research Report
  • [Journal Article] In-Situ Time-Resolved Dynamic Surface Events on the Pt/C Cathode in a Fuel Cell under Operando Conditions

    • Author(s)
      M.Tada, S.Murata, T.Asaoka, K.Hiroshima, K.Okumura, H.Tanida, T.Uruga, H.Nakanishi, S.Matsumoto, Y.Inada, M.Nomura, Y.Iwasawa
    • Journal Title

      Angew. Chem. Int. Ed. (In press)

    • Related Report
      2006 Annual Research Report
  • [Presentation] Aspects of Acid-Base Catalysis and Electron Transferon TiO_2(110)2007

    • Author(s)
      Y. Iwasawa
    • Organizer
      233th Am. Chem. Soc. National Meeting
    • Place of Presentation
      Chicago
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Presentation] Conceptual Integration of Homogeneous and Heterogeneous Catalyses for New Sustainable Green Processes on Catalyst Surfaces2007

    • Author(s)
      Y. Iwasawa
    • Organizer
      International Symposium on Relation Between Homogeneous and Heterogeneous Catalysis ISHHC 13)
    • Place of Presentation
      Berkeley, California
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Presentation] Atomic-level Structures and Mechanisms for Visible-light Photochemical and Thermal Reactions on TiO_2(110) and (001) Surfaces2006

    • Author(s)
      Y. Iwasawa
    • Organizer
      232nd Am. Chem. Soc. National Meeting
    • Place of Presentation
      San Francisco
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Presentation] Design and In-situ Characterization of Selective Catalysts for Green Processes", Symposium on Green Chemistry for Fuel2006

    • Author(s)
      Y. Iwasawa
    • Organizer
      232nd Am. Chem. Soc. National Meeting
    • Place of Presentation
      San Francisco
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Presentation] Photochemical and Thermal Reactions on TiO_2(110), TiO_2(001), and CeO_2(111)Surfaces Visualized by STM and NC-AFM2005

    • Author(s)
      Y. Iwasawa
    • Organizer
      Gordon Research Conference on Chemical Reactions on Surfaces
    • Place of Presentation
      Ventura, California
    • Year and Date
      2005-02-16
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Presentation] Photochemical and Thermal Reactions on TiP_2(110), TiO_2(001), and CeO_2(111) Surfaces Visualized by STM and NC-AFM2005

    • Author(s)
      Y. Iwasawa
    • Organizer
      Gordon Research Conference on Chemical Reactions on Surfaces
    • Place of Presentation
      Ventura, California
    • Year and Date
      2005-02-16
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Presentation] In Situ Catalyst Characterization by Time-Resolved DXAFS and SPM Associated with Designed Surfaces and Materials2005

    • Author(s)
      Y. Iwasawa
    • Organizer
      12^<th> International Symposium on Homogeneous and Heterogeneous Catalysis (ISHHC12)
    • Place of Presentation
      Florence, Italy
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Presentation] Time-Resolved Characterization of Selective Catalysis by DXAFS2005

    • Author(s)
      Y. Iwasawa
    • Organizer
      5^<th> International Conference on Oxidation Catalysis (WCOC)
    • Place of Presentation
      Sapporo
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Book] 表面工学ハンドブック2007

    • Author(s)
      唯美津木, 岩澤康裕
    • Publisher
      丸善株式会社(In press)
    • Related Report
      2006 Annual Research Report
  • [Book] Structure and Reaction Control at Catalyst Surfaces2006

    • Author(s)
      M. Tada, Y. Iwasawa
    • Total Pages
      27
    • Publisher
      Taylor & Francis
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Book] 新訂版・表面科学の基礎と応用-表面反応(通常の反応過程)(日本表面科学会編)2004

    • Author(s)
      岩澤康裕, 福井賢一
    • Total Pages
      6
    • Publisher
      エヌ・ティー・エス
    • Related Report
      2004 Annual Research Report
  • [Remarks] 「研究成果報告書概要(和文)」より

    • URL

      http://www.chem.s.u-tokyo.ac.jp/~yiwswlab/INDEX.htm

    • Related Report
      2006 Final Research Report Summary

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Published: 2004-04-01   Modified: 2018-03-28  

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