首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Temperature-Induced Route to Chaos in the H2O2-HSO_3~--S2O_3~(2-) Flow Reaction System
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Temperature-Induced Route to Chaos in the H2O2-HSO_3~--S2O_3~(2-) Flow Reaction System

机译:H2O2-HSO_3〜--S2O_3〜(2-)流动反应系统中温度诱导的混沌路径

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摘要

Low-frequency, high-amplitude pH-oscillations observed experimentally in the H2O2—HSO3~—SaO_3~(2-) flow reaction system at 21.0 °C undergo period-doubling cascades to chemical chaos upon decreasing the temperature to 19.0 °C in small steps. Period-4 oscillations are observed at 20.0 °C and can be calculated on the basis of a simple model. A reverse transition from chaos to high-frequency limit cycle oscillations is also observable in the reaction system upon decreasing further the temperature step by step to 15.0 °C. Period-2 oscillations are measured at 18.0 °C. Such a temperature-change-induced transition between periodic and chaotic oscillatory states can be understood by taking into account the different effects of temperature on the rates of composite reactions in the oscillatory system. Small differences in the activation energies of the composite reactions are responsible for the observed transitions. Temperature-change-induced period doubling is suggested as a simple tool for determining whether an experimentally observed random behavior in chemical systems is of deterministic origin or due to experimental noise.
机译:在H2O2-HSO3〜-SaO_3〜(2-)流动反应系统中于21.0°C进行实验观察到的低频,高振幅pH振荡,当温度降低至19.0°C时,经历周期性倍增的级联反应,形成化学混乱脚步。在20.0°C时观察到第4周期振荡,并可以基于简单模型进行计算。随着温度进一步逐步降低到15.0°C,在反应系统中也可以观察到从混沌到高频极限循环振荡的反向转变。第2周期的振荡是在18.0°C下测得的。通过考虑温度对振荡系统中复合反应速率的不同影响,可以理解这种温度变化引起的周期性和混沌振荡状态之间的过渡。复合反应的活化能的微小差异是所观察到的过渡的原因。建议将温度变化引起的周期加倍作为一种简单的工具,用于确定化学系统中实验观察到的随机行为是确定性起源还是由于实验噪声引起的。

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