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    二维膜电极组件电解池中CO2电催化还原模拟研究

    Simulation of CO2 Electrocatalytic Reduction in an Electrolyzer with 2D Membrane Electrode Modules

    • 摘要: 电催化CO2还原反应(eCO2RR)技术由于具有温和可控的反应条件且能够与清洁可再生能源想结合而存在广阔的发展前景。其中膜电极组件(MEA)电解池由于其紧密的结构、较高能量效率以及低欧姆损耗,具有的工业化应用的潜力。然而,现有的eCO2RR数字模型研究往往未能充分考虑溶液中酸碱平衡反应对电化学过程的影响,同时对气体扩散层(GDL)厚度和孔隙率对系统性能的作用也缺乏深入探讨。通过对MEA电解池进行几何建模,通过对流场、电化学反应、酸碱平衡反应、浓度场等多物理场的建立和耦合,成功搭建了一个二维MEA电解池的动态综合模型,并利用此模型探究了电解池中化学反应的不均匀分布现象、气体扩散层厚度以及孔隙率对MEA电解池系统的影响。模拟结果揭示了不平衡的酸碱反应导致阴极区域出现局部pH值波动,进而引发局部化学环境的变化,这导致了沿流道方向的催化剂层上电流密度的不均匀分布。此外,气体扩散层厚度和孔隙率的变化对气体传输和电极反应产生显著影响,从而改变了阴极流道中原料和产物的分布比例,并影响了产物的产量。本研究提出的二维动态MEA模型和对MEA电催化还原CO2性能的探究有助于后续CO2还原电解池的设计与开发。

       

      Abstract: The electrocatalytic CO2 reduction reaction (eCO2RR) technology is a promising area of research due to its mild and controllable reaction conditions and its ability to be combined with clean and renewable energy sources. In particular, membrane electrode assembly (MEA) electrolyzer have the potential for industrial application due to their compact structure, high energy efficiency and low ohmic losses. Nevertheless, existing numerical modelling studies of eCO2RR frequently fail to adequately consider the impact of acid-base equilibrium reactions in solution on the electrochemical processes. Furthermore, there is a paucity of in-depth analysis of the role of gas diffusion layer (GDL) thickness and porosity on the system performance. This paper presents a geometrical modelling of the MEA electrolyzer, which is then coupled with a dynamic and comprehensive model of

       

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