Atmospheric degradation mechanism of Z/E-CF3CF=CHCl, CF3CF=CCl2, and CF2=CFCl initiated by OH radicals using a smog chamber with long-path FT-IR at 298 K
Atmospheric degradation mechanism of Z/E-CF3CF=CHCl, CF3CF=CCl2, and CF2=CFCl initiated by OH radicals using a smog chamber with long-path FT-IR at 298 K
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使用具有 298K 长光程 FT-IR 的烟雾室，由 OH 自由基引发 Z/E-CF3CF=CHCl、CF3CF=CCl2 和 CF2=CFCl 的大气降解机制
DOI：
10.1016/j.atmosenv.2019.116991
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发表时间：
2019
期刊：
影响因子：
--
通讯作者：
Junji Mizukado
中科院分区：
文献类型：
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作者：
Qin Guo;Liang Chen;Junji Mizukado
本文用红外光谱仪研究了含氯氟烯烃Z/E-CF_3CF =CHCl、CF_3CF = CCl_2和CF_2 =CFCl在OH引发下的反应产物和反应机理。证明了氯原子是由含氯氟烯烃与OH自由基反应生成的，并且在实验期间观察到显著的加速。在Z/E-CF 3CF =CHCl反应中，相应的Cl引发反应产物被鉴定为CF 3CFClC（O）H，CF 3CF = CCl 2反应中，相应的Cl引发反应产物被鉴定为CF 3CFClC（O）Cl，CF2=CFCl反应中，相应的Cl引发反应产物被鉴定为CF2 ClC（O）F.讨论了Cl-释放对相关方法动力学研究的影响。通过对含氯氟烯烃与OH自由基和Cl原子的烟雾室反应产物的鉴定和定量分析，提出了含氯氟烯烃与OH自由基和Cl原子的烟雾室反应机理及其大气降解机理。还讨论了这些产品对大气的二次影响。
The products and mechanism for the OH-initiated reaction with the Cl-containing fluoroolefinsZ/E-CF3CF=CHCl, CF3CF=CCl2, and CF2=CFCl were investigated, using a smog chamber linked to a Fourier-transform infrared spectrometer. That Cl atoms were generated from Cl-containing fluoroolefin reactions with OH radicals was proven, and significant acceleration was observed during the experiments. The corresponding Cl-initiated reaction products were identified as CF3CFClC(O)H forZ/E-CF3CF=CHCl, CF3CFClC(O)Cl for CF3CF=CCl2, and CF2ClC(O)F for CF2=CFCl. The influence of Cl-release on the kinetic study using the relative method was also discussed. Mechanisms for smog chamber reactions between Cl-containing fluoroolefins and OH radicals and Cl atoms, and their atmospheric degradation mechanisms, were proposed, based on the identification and quantification of detected products. Secondary atmospheric impacts from these products were also discussed.