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亚氯酸盐-硫代硫酸盐非缓冲体系的动力学
引用本文:王舜,高庆宇,王新红,林娟娟,赖顺安,莫言学.亚氯酸盐-硫代硫酸盐非缓冲体系的动力学[J].物理化学学报,2003,19(8):762-765.
作者姓名:王舜  高庆宇  王新红  林娟娟  赖顺安  莫言学
作者单位:College of Chemical Engineering, China University of Mining and Technology, Xuzhou, 221008; Department of Chemistry and Material Science, Wenzhou Normal College, Wenzhou 325027
基金项目:国家自然科学基金(20103010),教育部优秀青年教师资助项目~~
摘    要:研究了亚氯酸盐-硫代硫酸盐反应体系在非缓冲条件下的复杂动力学行为.结果发现,在开放体系中反应的pH值和Pt电位存在准周期振荡分叉和混合模式振荡分叉通向混沌的过程,且pH峰与Pt电位峰反相位.当与起始浓度比相对较小时,随着流速的逐渐升高,体系的pH值和Pt电位从简单的小振幅振荡(S)经过准周期振荡分叉到混沌,最后回到简单大振幅振荡(L);而当与起始浓度比相对较高时,随着流速的降低,体系的pH值和Pt电位出现LS1、LS2、LS3…LSn的混合模式振荡,并在每对(LSn、LSn+1)振荡区间发现了LSn、LSn+1随机出现的非周期振荡行为.运用硫价态变化的一般动力学模型,模拟出了反应体系的混合模式振荡及非周期振荡.

关 键 词:准周期振荡  混合模式振荡  动力学模拟  
收稿时间:2003-01-07
修稿时间:2003年1月7日

Complex Kinetics of the Chlorite-Thiosulfate in an Unbuffered Reaction System
Wang Shun,Gao Qing-Yu Wang Xin-HongLin Juan-JuanLai Shun-An Mo Yan-Xue.Complex Kinetics of the Chlorite-Thiosulfate in an Unbuffered Reaction System[J].Acta Physico-Chimica Sinica,2003,19(8):762-765.
Authors:Wang Shun  Gao Qing-Yu Wang Xin-HongLin Juan-JuanLai Shun-An Mo Yan-Xue
Institution:College of Chemical Engineering, China University of Mining and Technology, Xuzhou, 221008; Department of Chemistry and Material Science, Wenzhou Normal College, Wenzhou 325027
Abstract:The complex kinetics of ClO 2--S 2 O 32-nonlinear reaction system in an unbu ffered solution has been investigated i n a CSTR.Both quasiperiodic and mixed-mode oscillations of pH and Pt potential were observed.At relatively lowNaClO 2 0/Na 2 S 2 O 3 0 ratio,the system changed from small-amplitude oscillations and quasip eri-odic oscillations to chaos and pure l arge-amplitude oscillations with i ncre asing the flow rate.At higher in itial concentration ratio,however,quasiperio dicity was given way to mixed-mode oscillations in which each period consists o f one large and n small peaks(LS n ).LS,LS 2 ,LS 3 ,...,LS n were obtained when the flow rate was decreased.For a narrow range of flow r ate between each pair of periodic re gions(LS n ,LS n+1 ),a region of aperiodic behavior,an apparently s tochastic mixture of LS n and LS n+1 ,was also observed.A general model based upon changes in the oxidation s t ate of sulfur in the presence of a gen eric oxidant simulated the mixed-mo de o scillations and aperiodic behavio r.
Keywords:Quasiperiodic oscillations  Mixed-mode oscillations  Dynamic simula tion  
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