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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Relative Rate and Product Studies of the Reactions of Atomic Chlorine with Tetrafluoroethylene, 1,2-Dichloro-1,2-difluoroethylene, 1,1-Dichloro-2,2-difluoroethylene, and Hexafluoro-1,3-butadiene in the Presence of Oxygen
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Relative Rate and Product Studies of the Reactions of Atomic Chlorine with Tetrafluoroethylene, 1,2-Dichloro-1,2-difluoroethylene, 1,1-Dichloro-2,2-difluoroethylene, and Hexafluoro-1,3-butadiene in the Presence of Oxygen

机译：存在下原子氯与四氟乙烯，1,2-二氯-1,2-二氟乙烯，1,1-二氯-2,2-二氟乙烯和六氟-1,3-丁二烯反应的相对速率和产物研究氧

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Rate tcoefficients k1-k3 have been measured for Cl atom reactions with CF2=CF2, CFCl=CFCl, and CCl2=CF2 relative to k(4) for CF2=CF-CF=CF2 at 293 +/- 2 K. k(4) was remeasured relative to Cl + ethane. Cl =was generated by UV photolysis of Cl-2, and other species were monitored by FT-IR spectroscopy. The measurements yield k(1) = (6.6 +/- 1.0) x 10(-11), k(2) = (6.5 +/- 1.0) x 10-11, and k3 = (7.1 +/- 1.1) x 10-11 cm3 molecule-1 s-1, respectively, and k4 = (8.0 +/- 1.2) x 10-11 cm3 molecule-1 s-1 is proposed. These results are discussed in the context of atmospheric chemistry. Subsequent chemistry in the presence of oxygen leads to oxygenated products that are identified via their IR spectra, and possible mechanisms are discussed. The yield of CF2O from C2F4 is 93 +/- 7%. Dichlorofluoroacetyl fluoride (CCl2FCFO) was observed as a product from CFClCFCl, and chlorodifluoroacetyl chloride (CClF2CClO) was observed from CCl2CF2 oxidation. C4F6 led to 66 +/- 5% CF2O and 38 +/- 3% OCF2CFC(F)=O. Reaction enthalpies and enthalpy barriers computed via CBS-QB3 theory help rule out some unfavorable mechanistic steps.
机译：相对于k（4），对于CF2 = CF-CF = CF2在293 +/- 2 K下，已经测量了CF2 = CF2，CFCl = CFCl和CCl2 = CF2的Cl原子反应的速率tcoefficient k1-k3.k（4相对于Cl +乙烷重新测量）。 Cl =是由Cl-2的紫外线光解产生的，其他种类则通过FT-IR光谱法监测。测量结果为k（1）=（6.6 +/- 1.0）x 10（-11），k（2）=（6.5 +/- 1.0）x 10-11和k3 =（7.1 +/- 1.1）x提出分别为10-11 cm3分子-1 s-1和k4 =（8.0 +/- 1.2）x 10-11 cm3分子-1 s-1。在大气化学的背景下讨论了这些结果。在氧气存在下的后续化学反应会导致氧化产物通过红外光谱进行鉴定，并讨论了可能的机理。 C2F4的CF2O产率为93 +/- 7％。观察到二氯氟乙酰氯（CCl2FCFO）是来自CFClCFCl的产物，而氯二氟乙酰氯（CClF2CClO）从CCl2CF2氧化中被观察到。 C4F6导致66 +/- 5％CF2O和38 +/- 3％OCF2CFC（F）= O。通过CBS-QB3理论计算出的反应焓和焓垒有助于排除一些不利的机理步骤。

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