Nonlinear instabilities in photochemical reactions

该计划旨在探索光化学反应中的非线性行为，并随后利用非线性动力学作为工具来深入了解这些复杂光化学反应中发生的基本过程。光化学反应在自然界中无处不在，从阳光对汽车尾气的作用到植物的光合作用。许多光化学过程涉及链式反应，这可能导致化学振荡和传播波等非线性不稳定性的发生。这项探索性研究有望发现一系列新的光介导化学振荡器，其中光在控制关键中间试剂的生产中发挥更关键的作用。这个程序将大大提高我们对摄动非线性动力学的理解。此外，本文还将开发利用非线性理论来深入了解1,4-苯醌和多巴胺等环状化合物的光化学反应的方法。这些方法也适用于其他光化学过程。我们将在间歇式反应器和连续流搅拌槽反应器中对1,4-苯醌-溴酸盐反应的光控非线性行为进行探索。反应之后将同时使用Pt和溴离子选择电极，再加上Hg|Hg2SO4|K2SO4参比电极。辐照将采用卤素光源，配备两根分叉的光纤。紫外/可见光谱法将用于分析中间种的进化。为了破译潜在的反应机制，反应混合物将进一步通过红外光谱，核磁共振和质谱分析。

This program aims to explore nonlinear behavior in photochemical reactions and to subsequently utilize nonlinear dynamics as a tool to gain insights into fundamental processes occurring in these complicated photochemical reactions. Photochemical reactions are ubiquitous in nature, ranging from the action of sunlight on car exhaust fumes to photosynthesis by plants. Many photochemical processes involve chain reactions, which can potentially result in the occurrence of nonlinear instabilities such as chemical oscillations and propagating waves. This exploratory research is expected to discover a series of new photo-mediated chemical oscillators, in which light plays a more critical role to exclusively control the production of key intermediate reagents. This program will significantly advance our understanding of perturbed nonlinear dynamics. In addition, methods of using nonlinear theory to gain insight into photochemical reactions of cyclic compounds such as 1,4-benzoquinone and dopamine will be developed here. These methods shall be applicable to other photochemical processes as well. Our exploration on light-controlled nonlinear behavior in the 1,4-benzoquinone-bromate reaction will be conducted in a batch reactor and in a continuously flow stirred tank reactor. Reactions will be followed simultaneously by a Pt and a bromide ion selective electrode, coupled with a Hg|Hg2SO4|K2SO4 reference electrode. Irradiation will be implemented with a halogen light source, equipped with two bifurcated optic fibers. UV/Vis spectroscopic method will be employed to analyze the evolution of intermediate species. To decipher the underlying reaction mechanisms, the reaction mixture will be further analyzed by Infrared Spectroscopy, NMR, and Mass Spectrometry.