物理化学学报 >> 2001, Vol. 17 >> Issue (06): 491-495.doi: 10.3866/PKU.WHXB20010604

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气相中H2O2与N2O反应机理的探讨

刘够生;宋兴福;于建国;钱旭红   

  1. 华东理工大学资源与环境工程学院,上海　200237
  • 收稿日期:2000-11-17 修回日期:2001-01-27 发布日期:2001-06-15
  • 通讯作者: 刘够生 E-mail:gs2000@jxnu.edu.cn

Theoretical Study on the Reaction Mechanism of H2O2 with N2O

Liu Gou-Sheng;Song Xing-Fu;Yu Jian-Guo;Qian Xu-Hong   

  1. School of Resource and Environmental Engineering, East China University of
  • Received:2000-11-17 Revised:2001-01-27 Published:2001-06-15
  • Contact: Liu Gou-Sheng E-mail:gs2000@jxnu.edu.cn

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摘要： 采用RHF/AM1方法研究了H2O2与N2O的反应机理.计算结果表明,该反应是多步反应,先后通过2个过渡态（TS1,TS3）,1个内旋转位垒（TS2）,2个中间体（IM1,IM2）.其中从反应物Re到TS1为整个反应的决速步骤,速控步骤的活化能为323.04 kJ•mol－1.整个反应为一放热反应,放出的热量为147.67kJ•mol－1.

关键词: AM1, 一氧化二氮, 反应机理, 量子化学

Abstract: Greenhouse effect has been received more and more attention in the field of environment protection recently. N2O is an important geenhouse effect gas, whose effect is 206 times stronger than that of CO2. Some researches show that beacuse of coupling relationship and competition effect between different trace gases, other trace gases can affect N2O′s life and ozone′s depletion speed in the atmosphere. In order to give an instructive theoretical reference to experimental researchers, AM1 molecular orbital methods using the restricted Hartree-Fock (RHF) calculation have been applied to investigate the mechanism of the reaction of H2O2 with N2O. The results show that this is a multistep reaction. Along the reaction path there are two transition states, one internal rotational barrier and two intermediates. The step from Re to IM1 is the ratecontrolling step, whose activation energy is 323.04 kJ•mol1. The whole reaction is exothermic, with the heat of formation equals to －147.67 kJ•mol－1.

Key words: AM1, N2O, Reaction mechanism, Quantum chemistry