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根据铂电极上硫化物电催化氧化的反应机理,本文提取动力学模型并利用数值模拟研究了N型负微分阻抗(N-NDR)振荡区域的电极表面时空反应动力学.在均相体系模拟中观察到电流简单振荡和复杂振荡,其来源于双电层电势自催化与传质限制和毒化物种吸附负反馈的相互耦合.为了更接近于真实体系,在模型中考虑了平行和垂直于电极表面两个方向的传质过程.模拟结果发现了与实验现象具有相同演化行为的复杂斑图,如行波和闪烁波;同时在传质耦合体系模拟中观察到双电层电势双臂螺旋波.本研究工作促进对电化学体系时空斑图的理解和预测.
According to the reaction mechanism of electrocatalytic oxidation of sulfide on platinum electrode, the kinetic model was extracted and the space-time reaction kinetics on the surface of N-type negative differential impedance (N-NDR) oscillation region was numerically simulated. In the homogeneous system simulation The simple oscillations of current and complex oscillations were observed, which originated from the mutual coupling of the electric double layer potential autocatalysis with mass transfer restrictions and the negative feedback of poisonous species adsorption. In order to be closer to the real system, parallel and perpendicular modes were considered in the model Two directions of mass transfer process.The simulation results show that the experimental images with the same evolutionary behavior of complex patterns, such as traveling wave and scintillation wave; At the same time in the mass-transfer coupling system simulation of double-layer potential bipolar spiral. This work promotes the understanding and prediction of the space-time pattern of electrochemical system.