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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Kinetic Study of the Reactions of Chlorine Atoms and CL_2~(.-) Radical Anions in Aqueous Solutions.II.Toluene,Benzoic Acid,and Chlorobenzene
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Kinetic Study of the Reactions of Chlorine Atoms and CL_2~(.-) Radical Anions in Aqueous Solutions.II.Toluene,Benzoic Acid,and Chlorobenzene

机译：水溶液中氯原子与CL_2〜（.-）自由基阴离子反应的动力学研究II。甲苯，苯甲酸和氯苯

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摘要

Laser and conventional flash photolysis of Na_2S_2O_8 aqueous solutions containing Cl~- ions were employed to investigate the reactions of chlorine atoms and Cl_2~(.-) radical ions with toluene, benzoic acid, and chlorobenzene. A mechanism is proposed which accounts for the faster decay of C1_2~(.-) in aqueous solutions containing increasing concentrations of the organic substrates. Interpretation of the experimental data is supported by kinetic computer simulations. Chlorine atoms react with the three substituted aromatics studied here almost with diffusion-controlled rate constants, k=(1.8+-0.3)X10~(10) M~(-1)s~(-1).The high reactivity observed for Cl atoms contrasts with that of the Cl_2~(-1)radical ions, for which the rate constant for its reactions with the substituted benzenes is <-1X10~6 M~(-1) s~(-1). The organic radicals produced from these reactions, as well as the nature of the reaction products are discussed. The observed results seem to support an addition mechanism yielding chlorocyclohexadienyl radicals (CI-CHD) as the most significant reaction channel following reaction of Cl atoms and the organic compounds. In air-saturated solutions, subsequent thermal reactions of CI-CHD radicals lead both to chlorination and oxidation of the aromatics.
机译：用激光和常规的闪蒸法对含Cl〜离子的Na_2S_2O_8水溶液进行了研究，研究了氯原子和Cl_2〜（.-）自由基离子与甲苯，苯甲酸和氯苯的反应。提出了一种机制，其解释了在包含增加的有机底物浓度的水溶液中，C1_2〜（.-）的快速衰减。动力学计算机仿真支持对实验数据的解释。氯原子与本文研究的三种取代的芳族化合物几乎以扩散控制的速率常数k =（1.8 + -0.3）X10〜（10）M〜（-1）s〜（-1）发生反应。原子与Cl_2〜（-1）自由基离子形成对比，Cl_2〜（-1）自由基与取代苯反应的速率常数<-1X10〜6 M〜（-1）s〜（-1）。讨论了由这些反应产生的有机基团以及反应产物的性质。观察到的结果似乎支持加成机理，该加成机理产生氯环己二烯基（CI-CHD）作为Cl原子与有机化合物反应之后最重要的反应通道。在空气饱和的溶液中，CI-CHD自由基的后续热反应会导致芳族化合物的氯化和氧化。

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