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金属ナノ構造体一分子複合系の赤外分光特性

Research Project

Project/Area Number 20043006
Research Category

Grant-in-Aid for Scientific Research on Priority Areas

Allocation TypeSingle-year Grants
Review Section Science and Engineering
Research InstitutionHokkaido University

Principal Investigator

大澤 雅俊  Hokkaido University, 触媒化学研究センター, 教授 (00108466)

Project Period (FY) 2008
Project Status Completed (Fiscal Year 2008)
Budget Amount *help
¥2,100,000 (Direct Cost: ¥2,100,000)
Fiscal Year 2008: ¥2,100,000 (Direct Cost: ¥2,100,000)
Keywords表面増強赤外吸収 / ナノ金属微粒子 / 表面振動分光 / 電極表面 / 電極触媒 / 水素発生 / 機能表面
Research Abstract

ナノ金属微粒子あるいはナノサイズの粗さをもつ金属表面に吸着した分子の赤外吸収強度が異常に増強される現象、表面増強赤外吸収(SEIRA)、の増強機構を電磁気学的観点から検討し、新たな理論モデルを構築した。このモデルは、従来のような有効誘電率近似を用いず、微粒子間の相互作用をより厳密に扱うとことに特徴がある。その結果、基板に誘起されるimage dipoleの影響を組み入れることが可能になった。この理論モデルは、増強度ならびにスペクトル形状が微粒子の形状、サイズ、密度に依存するという実験結果を適切に表現した。また、基板に誘起されるimage dipoleがSEIRAに大きく影響することを初めて明らかにした。モデル計算を通して、スペクトルを変形することなく増強度を最大にするナノ構造を明らかにした。
並行して、SEIRAを利用した固液界面反応計測を行い、Pt表面における硝酸化合物の還元反応とC1化合物の酸化反応、機能分子・錯体によるAu表面の機能化とその評価、電気二重層の再構成高速ダイナミクスの解析などを行い、いくつかの新しい知見を得た。最も重要な成果は、Ag電極を4, 4'-ビピリジンで修飾することにより、水の電気分解による水素発生が格段に促進されることを見出したことである。さらに、この反応が、単分子吸着した4, 4'-ビピリジンの酸化還元サイクルで触媒されていることを明らかにした。この結果から、分子の電子状態の制御により、さらに高活性な触媒システムが開発できる可能性があることを示唆された。さらなる検討は、ヒドロゲナーゼのような生体系における水素活性化機構の理解にも役立つものと期待される。

Report

(1 results)
  • 2008 Annual Research Report
  • Research Products

    (32 results)

All 2009 2008 Other

All Journal Article (15 results) (of which Peer Reviewed: 13 results) Presentation (16 results) Remarks (1 results)

  • [Journal Article] Fabrication of photochemical pattern on a self-assembled monolayer (SAM) of a ruthenium cluster under electrochemical control2009

    • Author(s)
      Y. Zhang
    • Journal Title

      Journal of Materials Chemistry 19

      Pages: 261-267

    • Related Report
      2008 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Recent progress in electrochemical surface science with atomic and Molecular Levels2009

    • Author(s)
      S. Ye
    • Journal Title

      Electrochemistry 77

      Pages: 1-20

    • Related Report
      2008 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 時間分解表面増強赤外分光による電極触媒反応解析2009

    • Author(s)
      G. Samjeske
    • Journal Title

      表面科学 30

      Pages: 68-74

    • Related Report
      2008 Annual Research Report
  • [Journal Article] Surface-enhanced infrared absorption spectroscopic studies of adsorbed nitrate, nitric oxide, and related compounds 1 : Reduction of adsorbed NO on a platinum electrode2008

    • Author(s)
      K. Nakata
    • Journal Title

      Langmuir 24

      Pages: 4352-4357

    • Related Report
      2008 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Surface-enhanced infrared absorption spectroscopic studies of adsorbed nitrate, nitric oxide, and related compounds 2 : Nitrate ion adsorption at a platinum electrode2008

    • Author(s)
      K. Nakata
    • Journal Title

      Langmuir 24

      Pages: 4358-4363

    • Related Report
      2008 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Formic acid electrooxidation on Pd in acidic solutions studied by surface-enhanced infrared absorption spectroscopy2008

    • Author(s)
      H. Miyake
    • Journal Title

      Physical Chemistry and Chemical Physics 10

      Pages: 3662-3669

    • Related Report
      2008 Annual Research Report
    • Peer Reviewed
  • [Journal Article] An unexpected enhancement in methanol electro-oxidation on an ensemble of Pt(111) nanofacets : A case of nanoscale single crystal ensemble electrocatalysis2008

    • Author(s)
      C. Susut
    • Journal Title

      Physical Chemistry and Chemical Physics 10

      Pages: 3712-3721

    • Related Report
      2008 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Electrochemical and infrared study of electro-oxidati6n of dimethyl ether (DME) on platinum polycrystalline electrode in acid solutions2008

    • Author(s)
      Y. Zhang
    • Journal Title

      Electrochimica Acta 53

      Pages: 6093-6103

    • Related Report
      2008 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Dynamics of double-layer restructuring on a Pt electrode covered by CO : Laser-induced potential transient measurement2008

    • Author(s)
      A. Yamakata
    • Journal Title

      Journal of Physical Chemistry C 112

      Pages: 11427-11432

    • Related Report
      2008 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Surface coordination of nitric oxide to a self-assembled monolayer of atriruthenium cluster : An in situ infrared spectroscopic study2008

    • Author(s)
      W. Zhou
    • Journal Title

      Langmuir 24

      Pages: 8027-8035

    • Related Report
      2008 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Hydrogen evolution reaction catalyzed by proton-coupled redox cycle of 4,4-binvridine monolaver adsorbed on silver electrodes2008

    • Author(s)
      T. Uchida
    • Journal Title

      Journal of American Chemical Society 130

      Pages: 10862-10863

    • Related Report
      2008 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Electrochemical behaviors of dimethyl ether on platinum single crystal Electrodes. Part I : Pt(111)2008

    • Author(s)
      L. Lu
    • Journal Title

      Journal of Electroanalytical Chemistry 619

      Pages: 143-151

    • Related Report
      2008 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Visible light responsive pristine metal oxide photocatalyst : Enhancement of activity by crystallization under hydrothermal treatment2008

    • Author(s)
      F. Amano
    • Journal Title

      Journal of American Chemical Society 130

      Pages: 17650-17651

    • Related Report
      2008 Annual Research Report
    • Peer Reviewed
  • [Journal Article] CO/Pt電極界面における電気二重層の構造ダイナミクス2008

    • Author(s)
      山方啓
    • Journal Title

      表面科学 29

      Pages: 526-531

    • Related Report
      2008 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 電極表面反応の表面増強赤外分光解析 : 裏から表を見る?2008

    • Author(s)
      大澤雅俊
    • Journal Title

      表面技術 59

      Pages: 68-74

    • Related Report
      2008 Annual Research Report
  • [Presentation] 電極界面におけるイオンの水和構造と破壊過程2009

    • Author(s)
      山方啓
    • Organizer
      電気化学会第76回大会
    • Place of Presentation
      京都大学
    • Year and Date
      2009-03-30
    • Related Report
      2008 Annual Research Report
  • [Presentation] Pt電極表面におけるCO酸化ダイナミクス : プレ酸化ピークの起源2009

    • Author(s)
      Gabor Samjeske
    • Organizer
      電気化学会第76回大会
    • Place of Presentation
      京都大学
    • Year and Date
      2009-03-30
    • Related Report
      2008 Annual Research Report
  • [Presentation] 時間分解赤外分光法を用いたGaN光電極の光励起ダイナミクス2009

    • Author(s)
      山方啓
    • Organizer
      第103回触媒討論会
    • Place of Presentation
      埼玉大学
    • Year and Date
      2009-03-30
    • Related Report
      2008 Annual Research Report
  • [Presentation] ビピリジン分子による電解水素発生の促進-有機分子による反応活性サイトの創成-2009

    • Author(s)
      内田太郎
    • Organizer
      第103回触媒討論会
    • Place of Presentation
      埼玉大学
    • Year and Date
      2009-03-30
    • Related Report
      2008 Annual Research Report
  • [Presentation] 電極界面における疎水性イオンの水和殻の構造とダイナミクス2009

    • Author(s)
      山方啓
    • Organizer
      日本化学会第89春季年会
    • Place of Presentation
      日大理工学部、船橋
    • Year and Date
      2009-03-29
    • Related Report
      2008 Annual Research Report
  • [Presentation] 和周波発生 (SFG) 分光法によるリチウムイオン電池界面の構造研究2009

    • Author(s)
      柳輝金
    • Organizer
      電気化学会第76回大会
    • Place of Presentation
      京都大学
    • Year and Date
      2009-03-29
    • Related Report
      2008 Annual Research Report
  • [Presentation] Ag電極に吸着した4,4'-ビピリジンの酸化還元サイクルが触媒する水素発生反応2009

    • Author(s)
      内田太郎
    • Organizer
      日本化学会第89春季年会
    • Place of Presentation
      日大理工学部、船橋
    • Year and Date
      2009-03-27
    • Related Report
      2008 Annual Research Report
  • [Presentation] ジメチルエーテル (DME) の電気化学的酸化反応のその場研究2009

    • Author(s)
      張一
    • Organizer
      電気化学会第76回大会
    • Place of Presentation
      京都大学
    • Year and Date
      2009-03-27
    • Related Report
      2008 Annual Research Report
  • [Presentation] Pt電極表面における水素発生反応の表面増強赤外分光解析2008

    • Author(s)
      大澤雅俊
    • Organizer
      第28回表面科学学術講演会
    • Place of Presentation
      早稲田大学
    • Year and Date
      2008-11-13
    • Related Report
      2008 Annual Research Report
  • [Presentation] Surface-enhanced infrared absorption spectroscopic studies of adsorbed nitrate and nitric oxide adsorbed on platinum electrodes2008

    • Author(s)
      K. Nakata
    • Organizer
      Pacific Rim Meeting on Electrochemical and Solid-State Science
    • Place of Presentation
      Honolulu, USA
    • Year and Date
      2008-10-16
    • Related Report
      2008 Annual Research Report
  • [Presentation] Dynamics of water molecules in the electric double layer studied by laser induced potential transient measurements2008

    • Author(s)
      A. Yamakata
    • Organizer
      Pacific Rim Meeting on Electrochemical and Solid-State Science
    • Place of Presentation
      Honolulu, USA
    • Year and Date
      2008-10-16
    • Related Report
      2008 Annual Research Report
  • [Presentation] Enhanced hydrogen evolution reaction on Ag electrodes catalyzed by proton-coupled redox cycles of 4,4'-bipyridine adsorbed on the surface2008

    • Author(s)
      T. Uchida
    • Organizer
      Pacific Rim Meeting on Electrochemical and Solid-State Science
    • Place of Presentation
      Honolulu, USA
    • Year and Date
      2008-10-15
    • Related Report
      2008 Annual Research Report
  • [Presentation] Structure of water at the Pt/acid interface : An infrared study2008

    • Author(s)
      M. Osawa
    • Organizer
      2008 Annual Meeting of International Society of Electrochemistry
    • Place of Presentation
      Seville, Spain
    • Year and Date
      2008-09-10
    • Related Report
      2008 Annual Research Report
  • [Presentation] Structure of water at the electrified platinum-water interface studied by surface-enhanced infrared absorption spectroscopy2008

    • Author(s)
      M. Osawa
    • Organizer
      The 25th European Congress on Surface Science
    • Place of Presentation
      Liverpool, UK
    • Year and Date
      2008-07-30
    • Related Report
      2008 Annual Research Report
  • [Presentation] Electrolysis of water on Ag electrode accelerated by the adsorption of 4,4'-bipyridine2008

    • Author(s)
      A. Yamakata
    • Organizer
      Catalysis for Hydrogen Energy Production & Utilization, A Post-Symposium of the 14th International Congress on Catalysis
    • Place of Presentation
      Gyeongju, Korea
    • Year and Date
      2008-07-22
    • Related Report
      2008 Annual Research Report
  • [Presentation] Potential oscillations in formaldehyde electrooxidation : A time-resolved surface-enhanced infrared study2008

    • Author(s)
      M. Osawa
    • Organizer
      4th Gerischer Symposium
    • Place of Presentation
      Berlin, Germany
    • Year and Date
      2008-06-25
    • Related Report
      2008 Annual Research Report
  • [Remarks]

    • URL

      http://www.cathokudai.acjp/osawai

    • Related Report
      2008 Annual Research Report

URL: 

Published: 2008-04-01   Modified: 2018-03-28  

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