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铂表面CO电氧化过程中的耗散孤子与逆火现象

Dissipative solitons and backfiring in the electrooxidation of CO on Pt.

作者信息

Bauer Philipp R, Bonnefont Antoine, Krischer Katharina

机构信息

Non-equilibrium Chemical Physics, Physik-Department, TU München, James-Franck-Str. 1, 85748 Garching, Germany.

Institut de Chimie de Strasbourg, UMR7177, CNRS et Université de Strasbourg, 4 rue Blaise Pascal, 67000 Strasbourg, France.

出版信息

Sci Rep. 2015 Nov 10;5:16312. doi: 10.1038/srep16312.

Abstract

Collisions of excitation pulses in dissipative systems lead usually to their annihilation. In this paper, we report electrochemical experiments exhibiting more complex pulse interaction with collision survival and pulse splitting, phenomena that have rarely been observed experimentally and are only poorly understood theoretically. Using spatially resolved in-situ Fourier transform infrared spectroscopy (FTIR) in the attenuated total reflection configuration, we monitored reaction pulses during the electrochemical oxidation of CO on Pt thin film electrodes in a flow cell. The system forms quasi-1d pulses that align parallel to the flow and propagate perpendicular to it. The pulses split once in a while, generating a second solitary wave in the backward moving direction. Upon collision, the waves penetrate each other in a soliton-like manner. These unusual pulse dynamics could be reproduced with a 3-component reaction-diffusion-migration model with two inhibitor species, one of them exhibiting a long-range spatial coupling. The simulations shed light on existence criteria of such dissipative solitons.

摘要

耗散系统中激发脉冲的碰撞通常会导致其湮灭。在本文中,我们报告了电化学实验,这些实验展示了更复杂的脉冲相互作用,包括碰撞存活和脉冲分裂,这些现象在实验中很少被观察到,在理论上也只是被初步理解。使用衰减全反射配置的空间分辨原位傅里叶变换红外光谱(FTIR),我们监测了流动池中Pt薄膜电极上CO电化学氧化过程中的反应脉冲。该系统形成准一维脉冲,这些脉冲与流动方向平行排列并垂直于流动方向传播。脉冲偶尔会分裂,在向后移动的方向上产生第二个孤立波。碰撞时,波以类似孤子的方式相互穿透。这些不寻常的脉冲动力学可以用一个包含两种抑制剂物种的三组分反应-扩散-迁移模型来重现,其中一种抑制剂表现出长程空间耦合。模拟揭示了这种耗散孤子的存在标准。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/af39/4639791/99a1378c5b4d/srep16312-f1.jpg

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