根据Berezin模型定量分析了胶束效应对阳离子三苯基甲基染料与水的反应速率的影响

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摘要

几种方法定量描述了表面活性剂胶束溶液对反应速率的影响。其中最常用的是Piszkiewicz的、Berezin的和伪相离子交换(PIE)模型。最后一个名字是由Bunton和Romsted开发的。Piszkiewicz的模型是根据质量作用定律来表示胶束形成的催化胶束,它由一些表面活性剂分子和一个底物组成。在我们之前的文章中,这个模型被用来解释阳离子三苯基甲基染料与水反应的动力学胶束效应,再次表明了这种方法的主要缺点。Berezin的模型是建立在胶束形成的另一种模型即伪相模型的基础上的,胶束对试剂的结合被认为是一种物质在两相之间的分布。在这项工作中,我们的目标是考虑Berezin的方法在非离子、阴离子、阳离子和两性离子表面活性剂的水系统中,孔雀石绿和亮绿阳离子与水分子作为亲核试剂的相互作用的适用性。总的来说,Berezin的模型在描述类似染料与氢氧根离子反应的胶束效应时表现良好。然而,该模型没有考虑到在体系中加入反应离子后,由于双电层压缩而引起的HO -离子局部浓度的变化,也没有考虑到HO -离子与表面活性剂阳离子头基的缔合常数。在这种情况下,当水被用作亲核试剂时,亲核试剂结合程度的问题可以用不同的方法来解决。PIE模型也是基于胶束化的伪相模型,但被胶束结合的底物被认为是一种化学计量比为1:1的结合,亲核试剂浓度以胶束中和程度为基础的局部浓度表示。考虑到后者,该方法不能应用于阳离子三苯基甲基染料与水反应的动力学胶束影响。
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Quantitative analysis of micellar effect on the reaction rate of cationic triphenylmethine dyes with water according to Berezin’s model
Several approaches quantitatively describe the effect of surfactant micellar solution on the reaction rate. The most used among them are Piszkiewicz’s, Berezin’s, and Pseudophase Ion-Exchange (PIE) models. The last-named was developed by Bunton and Romsted. Piszkiewicz’s model is based on representations of the micellization according to the mass action law with the formation of a catalytic micelle, which consists of some surfactant molecules and a substrate. In our previously paper, this model was used to explain the kinetic micellar effect on the reaction of cationic triphenylmethine dyes with water once again showed the main disadvantages of this approach. Berezin’s model is based on another model of micelle formation viz. the pseudophase model, and the binding of reagents by micelles is considered as the distribution of a substance between two phases. In this work, we aim to consider the applicability of Berezin’s approach for the interaction of malachite green and brilliant green cations with water molecule as a nucleophile in aqueous systems of nonionic, anionic, cationic, and zwitterionic surfactants. On the whole, Berezin's model performed well when applied to the description of the micellar effect on the reaction of similar dye with the hydroxide ion. However, it was revealed that this model does not take into account the change in the local concentration of the HO– ions due to a compression of the double electric layer upon addition of reacting ions to the system, as well as the constant of association of the HO– ions with cationic head groups of surfactant. In this case, when water is used as a nucleophile, the question of the degree of nucleophile binding can be solved differently. The PIE model is also based on a pseudophase model of micellization, but a substrate binding by micelles is considered as an association in a stoichiometric ratio of 1:1, and a nucleophile concentration is expressed in a local concentration based on the neutralization degree of micelles. Given the latter, its approach cannot be applied to the kinetic micellar influence on the reaction of cationic triphenylmethine dyes with water.
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