Abstract

Fast changes in the kinetic characteristics occur at the beginning of the transition processes of nonlinear chemical reactions, which are often not observed during nonstationary experiments. These periods of fast relaxations may carry important information about the mechanisms of complex reactions. The evolution of the period of fast relaxations of typical chemical reactions as they move away from equilibrium is studied in this paper. A three-level classification of the forms of nonequilibrium kinetic dependences with respect to the level of informativity is introduced. Nonmonotonic curves with bends (ravines, hills) have the maximum informativity, monotonic curves with bends (waves) have the average informativity, and monotonic curves without bends (descents, ascents) have the minimum informativity. The criterion of existence of the period of fast relaxations, during which the informative forms of the kinetic curves (ravines, hills, waves) exist, is formulated. It is shown that the states of false equilibrium can be observed during their study in which kinetic curves seem to be constant far from the equilibrium. The obtained results may be useful in the reconstruction of the mechanisms of chemical reactions.

中文翻译：

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化学反应快速弛豫的动力学特征

摘要

动力学特性的快速变化发生在非线性化学反应的过渡过程开始时，通常在非平稳实验中未观察到。这些快速弛豫时期可能携带有关复杂反应机理的重要信息。本文研究了典型化学反应在远离平衡状态时快速弛豫期的演变。引入了关于信息性水平的非平衡动力学依赖性形式的三级分类。带有弯曲（山沟，丘陵）的非单调曲线具有最大的信息性，带有弯曲（波浪）的单调曲线具有平均的信息性，而没有弯曲（下降，上升）的单调曲线具有最小的信息性。制定了快速弛豫期的存在准则，在此准则中存在动力学曲线的信息形式（沟壑，丘陵，波浪）。结果表明，在他们的研究中可以观察到虚假的平衡状态，其中动力学曲线似乎远离平衡是恒定的。获得的结果可能对重建化学反应的机理有用。