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Determination of the branching ratios between vibrational relaxation and reactive removal in collisions of free radicals and other molecules

自由基与其他分子碰撞时振动弛豫和反应去除之间支化比的测定

基本信息

批准号：
10640486
负责人：
YAMASAKI Katsuyoshi
金额：
$ 2.11万
依托单位：
NIIGATA UNIVERSITY
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (C)
财政年份：
1998
资助国家：
日本
起止时间：
1998 至 1999
项目状态：
已结题

项目摘要

A new method for determining the branching ratios between reactive removal and vibrational relaxation has been developed and experimental demonstration has been given. A mixture of OィイD23ィエD2/CHィイD24ィエD2/NィイD22ィエD2 in a flowing cell was photolyzed with a KrF (248nm) laser, and OH(XィイD12ィエD1ΠィイD2iィエD2, 0【less than or equal】υ【less than or equal】4) in the system were detected by laser-induced fluorescence (LIF). Time-dependent profiles of the LIF from the vibrational levels were recorded. The profiles were analyzed using integrated profiles method developed by our lab., and total removal rate constants for all the levels have been determined. The branching ratios between the following vibrational relaxation and reactive removal processes:OH(υ) + CHィイD24ィエD2 → OH(υ-1) + CHィイD24ィエD2 Vibrational relaxation→ Products Reactive removalhave been obtained using reported nascent vibrational distributions of OH in O(ィイD11ィエD1D) + CHィイD24ィエD2 reaction. It has been found that reactive removal process is accelerated with an increase in vibrational energies : k(υ=2)/k(υ=1)/k(υ=0) = 143/33/1.The new method of analysis was also adopted to HCO(υィイD21ィエD2υィイD22ィエD2υィイD23ィエD2) + 0ィイD22ィエD2 reactions. The LIF detection via BィイD4〜ィエD4ィイD12ィエD1A'-XィイD4〜ィエD4ィイD12ィエD1A' transition of HCO was employed to detect HCO. The highly sensitive detection method enabled experiments with parent molecule at very low concentrations. The rate constants for the reactions between HCO((000),(010),(001)) with molecular oxygen have been determined. We have succeeded in what we set out to do according to the plan for the project.

本文提出了一种测定反应性去除和振动弛豫分支比的新方法，并给出了实验验证。用KrF（248 nm）激光光解流动池中的O-[23]-[24]-[25]-[22]-[24]-[25]-[26]-[27]-[28]-[29]-[2记录了LIF的振动能级随时间变化的曲线。用本实验室开发的积分剖面法对剖面进行了分析，并测定了所有水平的总去除速率常数。用已报道的O（CH_（11）D_（11）+CH_（12）D_（24）D发现反应脱除过程随振动能的增加而加速：k（ε =2）/k（ε =1）/k（ε =0）= 143/33/1.新的分析方法也用于HCO（HCO D21 HCO D2 HCO D22 HCO D2 HCO D23 HCO D2）+ 0 HCO D22 HCO D2反应.通过HCO的B → D4 → D4 → D12 → D1 A '→ X → D4 → D12 → D1 A'跃迁的LIF检测用于检测HCO。高灵敏度的检测方法使得能够在非常低的浓度下用母体分子进行实验。测定了HCO（（000），（010），（001））与分子氧反应的速率常数。我们已经成功地完成了计划中的任务。