College of Chemical Engineering, China University of Mining and Technology, Xuzhou 221008 China.
J Phys Chem A. 2010 Jul 8;114(26):7014-20. doi: 10.1021/jp102010k.
We study the oxidation dynamics of thiosulfate ions by hydrogen peroxide in the presence of trace amounts of copper(II) using the reaction temperature as a control parameter in a continuous flow stirred tank reactor. The system displays period-doubling, aperodic, and mixed-mode oscillations at different temperatures. We are able to simulate these complex dynamics with a model proposed by Kurin-Csorgei et al. The model suggests that the Cu(2+)-containing term is not essential for the observed oscillations. We find small-amplitude and high-frequency oscillations in the catalyst-free experimental system. The reaction between H(2)O(2) and S(2)O(3)(2-) contains the core mechanism of the H(2)O(2)-S(2)O(3)(2-)-Cu(2+) and H(2)O(2)-S(2)O(3)(2-)-SO(3)(2-) oscillatory systems, while the Cu(2+) and SO(3)(2-) modulate the feedback loops so as to strengthen the oscillatory dynamics.
我们使用连续流搅拌槽反应器,以反应温度作为控制参数,研究了痕量铜(II)存在下过硫酸根离子与过氧化氢的氧化动力学。该系统在不同温度下表现出倍周期、非周期和混合模式振荡。我们能够使用 Kurin-Csorgei 等人提出的模型来模拟这些复杂的动力学。该模型表明,含 Cu(2+)的项对于观察到的振荡不是必需的。我们在无催化剂的实验系统中发现了小振幅和高频振荡。H(2)O(2)与 S(2)O(3)(2-)之间的反应包含 H(2)O(2)-S(2)O(3)(2-)-Cu(2+)和 H(2)O(2)-S(2)O(3)(2-)-SO(3)(2-)振荡系统的核心机制,而 Cu(2+)和 SO(3)(2-)调节反馈环,从而增强振荡动力学。