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铈-溴酸盐-4-氨基酚光反应中的混合模式和顺序振荡。

Mixed mode and sequential oscillations in the cerium-bromate-4-aminophenol photoreaction.

机构信息

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

出版信息

Chaos. 2013 Sep;23(3):033120. doi: 10.1063/1.4817514.

DOI:10.1063/1.4817514
PMID:24089956
Abstract

Cerium was introduced to the bromate-aminophenol photochemical oscillator to implement coupled autocatalytic feedbacks. Mixed mode and sequential oscillations emerged in the studied system, making it one of the few chemical oscillators known to support consecutive bifurcations in a batch system. The complex reaction behavior showed a strong dependence on the intensity of illumination supplied to the system. Removal of illumination during an oscillatory window affected both the frequency and amplitude of the oscillation but did not fully extinguish them, indicating that the cerium-bromate-4-aminophenol oscillator was photosensitive rather than photo-controlled. A moderate light intensity allowed for a slow evolution of the system, which proved to be critical for the emergence of transient complex oscillations. Variation of individual reaction parameters was carried out, which indicated that the development of complex oscillations occur in a narrow region and a phase diagram in the 4-aminophenol and sulfuric acid plane demonstrated this. Simulations provide strong support that transient complex oscillations observed experimentally arise from the coupling of two autocatalytic cycles.

摘要

铈被引入到溴酸盐-氨基酚光化学振荡器中,以实现偶联自催化反馈。在研究的系统中出现了混合模式和顺序振荡,这使得它成为少数已知的在批处理系统中支持连续分岔的化学振荡器之一。复杂的反应行为强烈依赖于系统所提供的光照强度。在振荡窗口期间去除光照会影响振荡的频率和幅度,但不会完全熄灭它们,这表明铈-溴酸盐-4-氨基酚振荡器是光敏的而不是光控的。适度的光强度允许系统缓慢演变,这对于出现瞬态复杂振荡至关重要。对单个反应参数进行了变化,这表明复杂振荡的发展发生在一个狭窄的区域,在 4-氨基酚和硫酸平面的相图中证明了这一点。模拟提供了强有力的支持,表明实验中观察到的瞬态复杂振荡是由两个自催化循环的耦合引起的。

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