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在封闭的亚铁催化贝洛索夫-扎博廷斯基反应中两种分岔状态的共存。

Coexistence of two bifurcation regimes in a closed ferroin-catalyzed Belousov-Zhabotinsky reaction.

作者信息

Wang Jichang, Zhao Jinpei, Chen Yu, Gao Qingyu, Wang Yumei

机构信息

Department of Chemistry and Biochemistry, The University of Windsor, Windsor, ON N9B 3P4, Canada.

出版信息

J Phys Chem A. 2005 Feb 24;109(7):1374-81. doi: 10.1021/jp0456279.


DOI:10.1021/jp0456279
PMID:16833454
Abstract

The ferroin-catalyzed Belousov-Zhabotinsky (BZ) reaction was studied in a batch reactor under anaerobic conditions and was found to evolve through two separated regimes of complex oscillations. Significantly, the two bifurcation regimes exhibited qualitatively different dependence on compositions of the reaction mixture, i.e., initial concentrations of bromate, sulfuric acid, malonic acid, and ferroin. The reaction temperature also showed opposite effects on the two bifurcation regimes, in which complexities of the first bifurcation regime were enhanced while oscillations in the second bifurcation regime became simpler as a result of decreasing temperature. Numerical simulations with a 12-variable model developed specifically for the ferroin-BZ system were able to reproduce transient complex oscillations observed in experiments. These calculations further illustrated that reactions such as ferroin and HOBr, ferroin and HBrO2, and ferriin and Br- were not essential in describing complex dynamics of the ferroin-BZ reaction.

摘要

在厌氧条件下,在间歇式反应器中研究了亚铁菲罗啉催化的贝洛索夫-扎博廷斯基(BZ)反应,发现该反应通过两种分离的复杂振荡模式进行。值得注意的是,这两种分岔模式对反应混合物的组成,即溴酸盐、硫酸、丙二酸和亚铁菲罗啉的初始浓度,表现出定性不同的依赖性。反应温度对这两种分岔模式也表现出相反的影响,其中随着温度降低,第一种分岔模式的复杂性增强,而第二种分岔模式中的振荡变得更简单。使用专门为亚铁菲罗啉-BZ系统开发的12变量模型进行的数值模拟能够重现实验中观察到的瞬态复杂振荡。这些计算进一步表明,诸如亚铁菲罗啉与HOBr、亚铁菲罗啉与HBrO2以及高铁菲罗啉与Br-等反应在描述亚铁菲罗啉-BZ反应的复杂动力学中并非必不可少。

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Coexistence of two bifurcation regimes in a closed ferroin-catalyzed Belousov-Zhabotinsky reaction.

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