物理化学学报 >> 2002, Vol. 18 >> Issue (06): 486-489.doi: 10.3866/PKU.WHXB20020602

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OH自由基与CO反应的研究

任丽;孔繁敖   

  1. 中国科学院化学研究所, 分子反应动力学国家重点实验室, 北京 100080
  • 收稿日期:2002-03-03 修回日期:2002-03-21 发布日期:2002-06-15
  • 通讯作者: 孔繁敖 E-mail:kong@mrdlab.icas.ac.cn

A Study of the Reaction of OH radical with CO by Time-resolved FTIR Spectroscopy

Ren Li;Kong Fan-Ao   

  1. State Key Laboratory of Molecular Reaction, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100080
  • Received:2002-03-03 Revised:2002-03-21 Published:2002-06-15
  • Contact: Kong Fan-Ao E-mail:kong@mrdlab.icas.ac.cn

摘要: 用时间分辨-傅立叶变换红外发射光谱法研究了OH自由基与CO的反应.OH自由基由248 nm的激光光解硝酸得到.在实验中首次观测到了产物CO2的非对称伸缩振动(ν3)的激发态.对CO2发射光谱的拟合结果显示,其振动态的布居在量子数v=2时最大 ,而最高振动量子数达到v=6.由实验得到的CO2振动布居与Schatz等人用全量子化计算该反应的中间物HOCO解离动力学得到的CO2布居结果能很好地吻合.

关键词: 时间分辨-傅立叶变换红外发射光谱, OH自由基, CO, CO2, 反应

Abstract: The reaction of OH radical with CO was investigated by time-resolved Fourier transform infrared (TR-FTIR) spectroscopy. OH radical was produced by laser photolysis of HNO3 at 248 nm. IR emission from vibrationally excited unsymmetric stretching mode (ν3) of product CO2 was observed for the first time (Fig.2). The simulated results for the IR emission spectrum of CO2 shows that the CO2 populates up to v=6 and the quantum number v=2 is the most populated vibration level (Fig.4). Comparison of the experimental distribution results of product CO2 with quantum or QCT calculation by Schatz and co-workers shows that experimental distributions agree well with the quantum predicting but is different from that of the QCT calculation. This consistency suggests that the SFH potential surface (Fig.1) is accurate and the quantum dynamics method but not QCT is proper approach for the chemical reaction involving H atom leaping.

Key words: TR-FTIR, OH radical, CO, CO2, reaction