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Experimental study of the reaction of molecules whose vibrational distribution is perturbed.

Research Project

Project/Area Number 02640349
Research Category

Grant-in-Aid for General Scientific Research (C)

Allocation TypeSingle-year Grants
Research Field 物理化学一般
Research InstitutionHiroshima University

Principal Investigator

SAITO Ko  Hiroshima Uni., Fac. Sci., Professor, 理学部, 教授 (00033853)

Project Period (FY) 1990 – 1991
Project Status Completed (Fiscal Year 1991)
Budget Amount *help
¥2,000,000 (Direct Cost: ¥2,000,000)
Fiscal Year 1991: ¥100,000 (Direct Cost: ¥100,000)
Fiscal Year 1990: ¥1,900,000 (Direct Cost: ¥1,900,000)
KeywordsChemical Kinetics / Unimolecular reaction / Shock Tube method / IR Laser absorption / Uibrational modo exitation / 衝撃浸管法 / 赤外線レ-ザ-吸収
Research Abstract

It is very important in the field of chemical kinetics to investigate that local-vibration-excited molecules behave different mannor from the usual molecules. Theortically, this is discussed on the basis of the coupling of the vibrational modes between the IRC and others. On the other hand, there are few report on the experimental study because of the difficulty of the obserbation. In this project, we tried to observe the reaction behavior by connecting the shock heating method and CO_2 infra-red laser shot. With this method it was found that acrylonitrile was decomposed after laser shot in the shock heated region. Since the laser power was less than 10mJ, laser shot merely perturbed the thermal disrtribution of the vibrational states.
The other method to produce local-vibration-excited molecules was the thermal decompositon of relatively large molecules. If ethyl vinyl ether is decomposed unimolecularly, acetaldehyde and ethylene are produced. The transition state of this reaction have a 6-centered structure and this structure suggests that the methyl group of the product aldehyde is strongly excited in the rotation or H-C-H bending mode. Therefore, it is expected that the acetaldehyde produced in this monnor behaves unusual kinetics. In fact, we found that this aldehyde decomposed with very large rate constants compared with the usual value.
Thus, we ascertained that the local excitation of vibrations affected sensitively the unimolecular decomposition rate.

Report

(3 results)
  • 1991 Annual Research Report   Final Research Report Summary
  • 1990 Annual Research Report
  • Research Products

    (16 results)

All Other

All Publications (16 results)

  • [Publications] K.Saito: "Thermal decomposition of ethyl acetate.Branching ratio of the competing paths in the pyrolysis of the produced acetic acid." Chem.Phys.Letters. 170. 385-388 (1990)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] M.Koshi: "Reactions of N( ^4S) atoms with NO and H_2" J.Chem.Phys.93. 8703-8708 (1990)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] K.Shimofuji: "Unimolecular thermal decomposition of ethyl vinyl ether and the consecultive thermal reaction of the intermediary product acetaldehyde:Shock wave experiment and ab initio calculation." J.Phys.Chem.95. 155-165 (1991)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] K.Saito: "Unimolecular reaction of acetaldoxime at high temperatures:Experiments and calculations" J.Phys.Chem.

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] K.Saito: "Vibrational states of the carbon monoxide produced via successive unimolecular decomposition of relatively large molecules" Proc.18th Int.Symp.on Shock Waves. (1992)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] K. Saito, T. Sasaki, I. Yoshinobu and A. Imamura: "Thermal decomposition of ethyl acetate. Branching ratio of the competing paths in the pyrolysis of the produced acetic acid." Chem. Phys. Lett.170. 385-388 (1990)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] K. Shimofuji, K. Saito and A. Imamura: "Unimolecular thermal decomposition of ethyl vinyl ether and the consecutive thermal reaction of the intermediary product acetaldehyde : Shock wave experiment and ab initio calculation" J. Phys. Chem.,. 95. 155-165 (1991)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] M. Koshi, M. Yoshimura, K. Fukuda, H. Matsui, K. Saito, M. Watanabe, A. Imamura and Congxia Chen: "Reactions of N( ^4S) atoms with NO and H_2" J. Chem. Phys.,. 93. 8703-8708 (1990)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] K. Saito, M. Watanabe, K. Adachi, M. Sugimoto, K. Okada and G. Sasaki: "Vibrational states of the carbon monoxide produced via successive unimolecular decomposition of relatively large molecules" Proc. 18th Int. Sympo. on Shock Waves,. (1991)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] K. Saito, K. Okada and A. Imamura: "Unimolecular reaction of acetaldoxime at high temperatures : Experiments and calculations." J. Phys. Chem.

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] K.Saito: "Unimolecular reaction of acetaldoxime at high temperatures:Experiments and calculations" J.Phys.Chem.

    • Related Report
      1991 Annual Research Report
  • [Publications] K.Saito: "Vibrational states of the carbon monoxide produced viasuccessive unimolecular decomposition of relatively large molecules" Proc.18th Int.Symp.on Shock Waves. (1992)

    • Related Report
      1991 Annual Research Report
  • [Publications] K.Saito: "Thermal decomposition of ethyl acetate.Brenching ratio of the competing paths in the pyrolysis of the produced acetic acid." Chem.Phys.Letter. 170. 385-388 (1990)

    • Related Report
      1990 Annual Research Report
  • [Publications] K.Shimofuji: "Unimolecular thermal decomposition of ethyl vinyl ether and the consecutive thermal reaction of the intermediary product acetaldehyde:Shock wave experiment and ab initio calculation." J.Phys.Chem.95. 155-165 (1991)

    • Related Report
      1990 Annual Research Report
  • [Publications] M.Koshi: "Reactions of N( ^4S)atoms with NO and H_2" J.Chem.Phys.93. 8703-8708 (1990)

    • Related Report
      1990 Annual Research Report
  • [Publications] K.Saito: "Unimolecular reaction of acetaldoxime at high temperatures:Experiments and calculations" J.Phys.Chem.

    • Related Report
      1990 Annual Research Report

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Published: 1990-04-01   Modified: 2016-04-21  

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