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Peculiar nitrogen desorption on rhodium surfaces and the decomposition mechanism of nitrogen oxides

Research Project

Project/Area Number 13640493
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeSingle-year Grants
Section一般
Research Field Physical chemistry
Research InstitutionHokkaido University

Principal Investigator

MATSUSHIMA Tatsuo  Hokkaido Univ., Catalysis Resarch Center, Professor, 触媒化学研究センター, 教授 (30002116)

Project Period (FY) 2001 – 2002
Project Status Completed (Fiscal Year 2002)
Budget Amount *help
¥800,000 (Direct Cost: ¥800,000)
Fiscal Year 2002: ¥800,000 (Direct Cost: ¥800,000)
Keywordsnitrogen oxide / rhodium catalyst / product desorption process / nitrous oxide / decomposition / inclined desorption / nitrogen desorption / angular distribution of desorption / 窒素酸化物 / 分解機構
Research Abstract

Improvements of cooling performance and pumping rates ; A sample crystal in the angle-resolved thermal desorption apparatus was successfully improved to be cooled from 90K to 50K. The pumping rate was increased about 5 times and high enough to reduce the background signal level to one fifth.
N_2O decomposition on clean Rh(110) ; N_2O is already decomposed from 60 K and yields five N_2 desorption peaks in the range of 70-170 K. β_1-N_2 peaking at around 165 K shows a cosine distribution, indicating desorption from N_2 trapped once on the surface after N_2O dissociation. Β_2-N_2 peaked at 140 K and β_ 3-N_2 at 120K. These peaks appeared at higher N_2O exposures and collimate at 68 degrees from the surface normal in the plane in the [001] direction. On the other hand, both β_4-N_2 and β_5-N_2 were observed at small N_2O exposures. These collimate 68 degrees off the surface normal into the [001] direction.
N_2 desorption is sensitive to the amount of residual surface oxygen. The amount was controlled by selecting pre-heating temperature, N_2O is not decomposed when the pre-heating is below 1000 K. After the pre-heating at 1100 K, N_2O is decomposed at 100-170 K, emitting N_2 collimated at around 30 degrees along the [001] direction. A (1x2) missing-row structure was observed by LEED. The 30 degree component was proposed to be formed on declining terraces on the missing-row structure.
The orientation of adsorbed N_2O on Rh(110) was examined at 70 K by near-edge X-ray absorption fine structure. N_2O is partly dissociated at 70 K at low N_2O exposures. At higher N_2O coverage, two adsorption forms, standing and lying, were proposed.
Similar results were obtained on Pd(110) for N_2O decomposition and adsorption.

Report

(3 results)
  • 2002 Annual Research Report   Final Research Report Summary
  • 2001 Annual Research Report
  • Research Products

    (21 results)

All Other

All Publications (21 results)

  • [Publications] 大野佑一: "Product desorption dynamics in explosive NO+CO reaction on Pt(100)"Chemical Physics Letters. 373. 161-166 (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] 劉 素文: "N_2 desorption in the decomposition of adsorbed N_2O, on oxygen-covered Rh(110)"J. Physical Chemistry B. (印刷中). (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Rzeznicka Izabela: "Bi-directional CO_2 desorption in steady-state CO oxidation on Rh(110)"J. Physical Chemistry B. (印刷中). (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Kobal Ivan: "Surface-nitrogen Removal Studied from Desorption Dynamics"Trends in Physical Chemistry. (印刷中). (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] 胡 玉海: "Different CO_2 collimation on stepped Pt(112); A comparison of NO(a)+CO(a) and CO(a)+O(a) reactions"Surface Science. 526. 159-165 (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Kokalj Anton: "A DFT study of adsorbed N_2O on Pd(110)"J. Phys. Chem. B. 107. 2741-2747 (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Ohno Yuichi: "Product desorption dynamics in explosive NO+CO reaction on Pt(100)"Chemical Physics Letters. in press. (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Liu Suwen: "N_2 deporption in the decomposition of adsorbed N_2O on oxygen-covered Rh(110)"J. Physical Chemistry. in press. (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Rzeznicka Izabela: "Bi-directional CO_2 desorption in steady-state CO oxidation on Rh(110)"J. Physical Chemistry B. in press. (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Hu Yuhai: "Different CO_2 collimation on stepped Pt(112) ; A comparison of NO(a)+CO(a) and CO(a)+O(a) reactions"Surface Science. 526. 159-165 (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Kokalj Anton: "A DFT study of adsorbed N_2O on Pd(110)"J. Phys. Chem. B. 107. 2741-2747 (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] 大野佑一: "Product desorption dynamics in explosive NO+CO reaction on Pt(100)"Chemical Physics Letters. (印刷中). (2003)

    • Related Report
      2002 Annual Research Report
  • [Publications] 劉 素文: "N_2 desorption in the decomposition of adsorbed N_2O on oxygen-covered Rh(110)"J.Physical Chemistry. (印刷中). (2003)

    • Related Report
      2002 Annual Research Report
  • [Publications] Rzeznicka Izabela: "Bi-directional CO_2 desorption in steady-state CO oxidation on Rh(110)"J.Physical Chemistry. (印刷中). (2003)

    • Related Report
      2002 Annual Research Report
  • [Publications] Kobal Ivan: "Surface-nitrogen Removal Studied from Desorption Dynamics"Trends in Physical Chemistry. (印刷中). (2003)

    • Related Report
      2002 Annual Research Report
  • [Publications] 胡 玉海: "Different CO_2 collimation on stepped Pt(112) ; A comparison of NO(a)+CO(a) and CO(a)+O(a) reactions"Surface Science. 526. 159-165 (2003)

    • Related Report
      2002 Annual Research Report
  • [Publications] Kokalj Anton: "A DFT study of adsorbed N_2O on Pd(110)"J. Phys. Chem.. (印刷中). (2003)

    • Related Report
      2002 Annual Research Report
  • [Publications] Anton Kokalj: "Orientation of N_2O molecule on Pd(110) surface"Surface Science. (印刷中). (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] Tatsuo Matsushima: "Decomposition of nitrogen oxides on palladium and angle-resolved measurements of desorbing products"Catalysis Surveys from Japan. 5. 71-80 (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] Ivan Kobal: "Site identification and angle-resolved measurements of desorbing surface reaction products under steady-state conditions"Recent research developments in physical chemistry. (印刷中). (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] Hideyuki Horino: "Ad-molecule orientation and photo-/thermal-induced surface-aligned desorption"Topics in Catalysis. 18(1). 21-26 (2002)

    • Related Report
      2001 Annual Research Report

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Published: 2002-04-01   Modified: 2016-04-21  

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