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通过与 OH-自由基的反应研究 CF₃CH=CH₂、CF₃CF=CH₂ 和 CF₃CF=CF₂ 的反应机理、动力学和大气命运:CVT/SCT/ISPE 和混合 meta-DFT 方法。

Mechanism, kinetics and atmospheric fate of CF₃CH=CH₂, CF₃CF=CH₂, and CF₃CF=CF₂ by its reaction with OH-radicals: CVT/SCT/ISPE and hybrid meta-DFT methods.

机构信息

Department of Chemistry, Indian Institute of Technology Madras, Chennai 600036, India.

Department of Chemistry, Indian Institute of Technology Madras, Chennai 600036, India.

出版信息

J Mol Graph Model. 2014 Mar;48:60-9. doi: 10.1016/j.jmgm.2013.12.003. Epub 2013 Dec 11.

Abstract

The dual level direct dynamic study is carried out for the reactions of CF₃CH=CH₂, CF₃CF=CH₂ and CF₃CF=CF₂ with hydroxyl radicals. The dynamic calculations are performed using the variational transition state theory (VTST) with interpolated single-point energies (ISPE) method at M06-2X/MG3S//M06-2X/6-31+G(d,p) level of theory. All the possible reactions such as abstraction and addition-elimination pathways are explored for the title reactions. The temperature dependent rate coefficients using canonical variational transition state theory with small curvature tunneling for the reaction of OH radicals with test molecules over the temperature range of 200-3000 K are computed. The predicted rate coefficients (in 10⁻¹² cm³ molecule⁻¹ s⁻¹) using CVT/SCT/ISPE methodology for the reaction of CF₃CH=CH₂, CF₃CF=CH₂ and CF₃CF=CF₂ with OH radicals are 1.48, 1.02 and 1.77, respectively, are in good agreement with reported ones at 298 K. The atmospheric lifetimes for the test molecules CF₃CH=CH₂, CF₃CF=CH₂ and CF₃CF=CF₂ are calculated at 277 K to be 8, 11 and 6 days, respectively. Global warming potentials are also reported for the different time horizon of 20, 100 and 500 years.

摘要

对 CF₃CH=CH₂、CF₃CF=CH₂ 和 CF₃CF=CF₂ 与羟基自由基的反应进行了双水平直接动态研究。动力学计算使用变分过渡态理论 (VTST) 与插值单点能 (ISPE) 方法在 M06-2X/MG3S//M06-2X/6-31+G(d,p) 理论水平上进行。对于标题反应,探索了所有可能的反应途径,如抽提和加成消除途径。使用正则变分过渡态理论和小曲率隧道方法计算了 OH 自由基与测试分子在 200-3000 K 温度范围内的反应的温度相关速率系数。使用 CVT/SCT/ISPE 方法预测的 CF₃CH=CH₂、CF₃CF=CH₂ 和 CF₃CF=CF₂ 与 OH 自由基反应的速率系数(在 10⁻¹² cm³分子⁻¹ s⁻¹)分别为 1.48、1.02 和 1.77,与 298 K 时报道的值吻合较好。测试分子 CF₃CH=CH₂、CF₃CF=CH₂ 和 CF₃CF=CF₂ 在 277 K 时的大气寿命分别计算为 8、11 和 6 天。还报告了不同时间跨度(20、100 和 500 年)的全球变暖潜能值。

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