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Detection, role and utilization of excited molecules in catalytic reaction by means of IR chemiluminescence

Research Project

Project/Area Number 17560679
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeSingle-year Grants
Section一般
Research Field Catalyst/Resource chemical process
Research InstitutionUniversity of Tsukuba

Principal Investigator

KUNIMORI Kimio  University of Tsukuba, Graduate School of Pure and Applied Sciences, Professor (60132990)

Co-Investigator(Kenkyū-buntansha) TOMISHIGE Keiichi  University of Tsukuba, Graduate School of Pure and Applied Sciences, Associate Professor (50262051)
Project Period (FY) 2005 – 2007
Project Status Completed (Fiscal Year 2007)
Budget Amount *help
¥3,680,000 (Direct Cost: ¥3,500,000、Indirect Cost: ¥180,000)
Fiscal Year 2007: ¥780,000 (Direct Cost: ¥600,000、Indirect Cost: ¥180,000)
Fiscal Year 2006: ¥600,000 (Direct Cost: ¥600,000)
Fiscal Year 2005: ¥2,300,000 (Direct Cost: ¥2,300,000)
KeywordsIR chemiluminescence / Vibrationally-excited molecules / Dynamics of catalytic reaction / Molecular beam of excited methane / Production of CO and H_2 / メタン・エタン励起分子線
Research Abstract

(1) Dynamics of catalytic reactions by measurement of IR emission of the vibrationally-excited product molecules
(1-1) CO+O_2 reaction on Pd (110), Pd (111)
Analysis method using intensities of IR emission was proposed, and changes in vibrational temperatures were measured with increasing surface temperature.
(1-2) CO+NO reaction on Pd (110), Pd (111)
Large structure-sensitivity in the activity of the CO+NO reaction was found for the first time. NO Dissociation does not take place on Pd (111), and nascent oxygen from NO is formed on Pd (110) because NO dissociation is limited.
(1-3) CO+0_2 reaction on Pt (110), Pt (111)
Activity was higher on Pt (110) than on Pt (111). Changes in vibrational temperatures were observed due to the reconstruction of (l x l) into (1 x 2) on Pt (110).
(2) Direct catalytic partial oxidation of CH_4 and C_2H_6 using heatable and seeded molecular beam technique
(2-1) The promoting effect of energetic activation of a methane molecular beam: production of syngas
CO+H_2 (in particular H_2) were produced selectively during steady-state CH_4+O_2 reaction on Pt by exciting methane. The reaction also takes place on Rh by reducing O_2.
(2-2) Comparative study between methane and ethane in the catalytic paratial reaction on Pt and Rh
Based on the results of the reaction order measurements one possible explanation for the promotion is that energetically activated methane and ethane react with adsorbed oxygen and produce methoxy and ethoxy species, which are regarded as precursors for hydrogen formation.

Report

(4 results)
  • 2007 Annual Research Report   Final Research Report Summary
  • 2006 Annual Research Report
  • 2005 Annual Research Report
  • Research Products

    (19 results)

All 2007 2006 2005

All Journal Article (17 results) (of which Peer Reviewed: 3 results) Presentation (2 results)

  • [Journal Article] CO oxidation on Pd(111), Pt(111) by IR chemiluminescence2007

    • Author(s)
      中尾憲治、冨重圭一、国森公夫
    • Journal Title

      Surface Science 601

      Pages: 3796-3800

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] Comprativ study between methane and ethane in catalytic partial oxidation over Pt and Rh foils using molecular-beam technique2007

    • Author(s)
      佐々木敏彰、冨重圭一、国森公夫
    • Journal Title

      Applied Catalysis, A: General 328

      Pages: 140-149

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] CO oxidation on Pd(111), Pt(111) and Rh(111) studied by IR chemiluminescence2007

    • Author(s)
      K. Nakao, K. Tomishige, K. Kunimori
    • Journal Title

      Surface Science 601

      Pages: 3796-3800

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Journal Article] Comparative study between methane and ethane in catalytic partial oxidation over Pt and Rh foils using molecular-beam technique2007

    • Author(s)
      T. Sasaki, K. Tomishige, K. Kunimori
    • Journal Title

      Applied Catalysis, A 328

      Pages: 140-149

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Journal Article] CO oxidation on Pt(111) and Pt(110) surfaces studied by IR chemilumincescence spectroscopy2007

    • Author(s)
      中尾 憲治、国森 公夫等
    • Journal Title

      Surface Science 601

      Pages: 3796-3800

    • Related Report
      2007 Annual Research Report
  • [Journal Article] Comparative study between methane and ethane in catalytic partialoxidation over Pt and Rh foils using molecular-beam technique2007

    • Author(s)
      佐々木 俊彰、国森 公夫等
    • Journal Title

      Applied Catalysis, A: General, 328

      Pages: 140-149

    • Related Report
      2007 Annual Research Report
  • [Journal Article] Comparative Study in CO oxidation by O_2 NO and N_2O on Pd(110)2006

    • Author(s)
      中尾憲治、冨重圭一、国森公夫
    • Journal Title

      Surface Science 600

      Pages: 4221-4227

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] Comparative Study in CO oxidation by O_2, NO and N_2O on Pd(110)2006

    • Author(s)
      K. Nakao, K. Tomishige, K. Kunimori
    • Journal Title

      Surface Science 600

      Pages: 4221-4227

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Journal Article] IR chemilumincesscence study of CO2 formed during steady-state CO oxidation on Pt(111) and Pt(110) surfaces2006

    • Author(s)
      中尾 憲治, 国森 公夫, 等
    • Journal Title

      Journal of the Surface Science Society of Japan 24

      Pages: 461-467

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Promoting effect of energetic activation of methane molecular-beam in direct catalytic partial oxidation of methane2006

    • Author(s)
      佐々木 俊彰, 国森 公夫, 等
    • Journal Title

      Chemical Communications

      Pages: 3821-3823

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Comparative study of CO_2 formation in CO oxidation by O_2,NO and N_2O on Pd(110) surface using infrared chemilunescence2006

    • Author(s)
      中尾 憲治, 国森 公夫, 等
    • Journal Title

      Surface Science 600

      Pages: 4221-4227

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Reaction mechanism and structure of activated complex of CO_2 formation in CO oxidation on Pd(110) and Pd(111) surfaces2006

    • Author(s)
      中尾憲治, 国森 公夫等
    • Journal Title

      Catalysis Today 111

      Pages: 316-321

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Infrared chemiluminescence study of CO + O_2 reaction on Pd(110) : Activated complex of CO_2 formation at high CO coverage2005

    • Author(s)
      中尾憲治, 国森 公夫等
    • Journal Title

      Chemical Physics Letters 410

      Pages: 86-89

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Vibrationally excited CO_2 formed in CO + NO reaction on Pd(110) surface in high surface temperature range2005

    • Author(s)
      中尾憲治, 国森 公夫等
    • Journal Title

      Catalysis Letters 103

      Pages: 179-184

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Structure of activated complex of CO_2 formation in CO + O_2 reaction on Pd(110) and Pd(111)2005

    • Author(s)
      中尾憲治, 国森 公夫等
    • Journal Title

      J.Physical Chemistry, B 109

      Pages: 17553-17559

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Infrared chemiluminescence study of CO_2 formation in CO + NO reaction on Pd(110) and Pd(111)2005

    • Author(s)
      中尾憲治, 国森 公夫等
    • Journal Title

      J.Physical Chemistry, B 109

      Pages: 17579-17586

    • Related Report
      2005 Annual Research Report
  • [Journal Article] IR chemiluminescence probe of the vibrational energy distribution of CO_2 formed during steady-state CO oxidation on Pt(110) and Pt(111)2005

    • Author(s)
      中尾憲治, 国森 公夫等
    • Journal Title

      J.Physical Chemistry, B 109

      Pages: 24002-24007

    • Related Report
      2005 Annual Research Report
  • [Presentation] 赤外線化学発光法を用いた Rh (110)および Rh (111)上のCO+NO 反応2007

    • Author(s)
      渡辺整・冨重圭-・国森公夫
    • Organizer
      触媒学会
    • Place of Presentation
      北海道大学理学部等
    • Year and Date
      2007-09-20
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] CO+NO reaction on Rh(110) and Rh(111) studied by IR chemiluminescence2007

    • Author(s)
      O. Watanabe, K. Tomishige, K. Kunimori
    • Organizer
      100th meeting of Catalysis Society of Japan
    • Place of Presentation
      Hokkaido University
    • Year and Date
      2007-09-20
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary

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Published: 2005-04-01   Modified: 2016-04-21  

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