过氧化氢氧化硫氧化合物的动力学行为与机理

Dynamical Behavior and Mechanism of the Oxidation of Oxygen-Sulfur Compounds by Hydrogen Peroxide

实验研究了过氧化氢氧化硫氧化合物反应体系在封闭搅拌状态下表现出的复杂动力学行为,并提出了9步反应机理的过氧化氢氧化硫代硫酸盐反应体系的改进模型.它包含连四硫酸盐水解反应步骤:2S4O62-+6OH-→3S2O32-+2SO32-+3H2O,不仅能够模拟多个过氧化氢-硫氧化合物反应体系的pH单峰振荡和准振荡行为,而且能够再现过氧化氢-亚硫酸盐-硫代硫酸盐非缓冲体系在开放条件下的简单周期振荡、倍周期振荡和混沌等复杂动力学行为.

The complex dynamics of the oxidations of oxygen-sulfur compounds by hydrogen peroxide were investigated in both closed and open systems. A 9-step mechanism modified model is suggested, in which it is essential to include the reaction 2S4O6^2- ＋ 6OH^-→3S2O3^2- ＋ 2SO3^2-＋ 3H2O. The mechanism not only agrees with batch experimental results of hydrogen peroxide-oxygensulfur compound systems, but also reproduces simple oscillations, double-period oscillations and chaos observed in the H2O2-Na2SO3-Na2S2O3 open system.