Sharma Raghunandan, Andersen Shuang Ma
Department of Chemical Engineering, Biotechnology and Environmental Technology , University of Southern Denmark , Campusvej 55 , DK-5230 Odense M , Denmark.
ACS Appl Mater Interfaces. 2018 Nov 7;10(44):38125-38133. doi: 10.1021/acsami.8b14622. Epub 2018 Oct 24.
Large-scale applications of polymer electrolyte membrane fuel cells (PEMFCs) are throttled primarily by high initial cost and durability issues of the electrodes, which essentially consist of the nanoparticulate catalysts (e.g., Pt) having accessibility to electrons (e), protons (H), and fuel/oxidant through catalyst support, polymer electrolyte ionomer, and porous gas diffusion layer, respectively. Hence, to achieve high electrode performance in terms of activity and/or durability, understanding and optimization of the catalyst/support and catalyst/ionomer interfaces are of significant importance. Present study demonstrates an alternative route to inspect the catalyst/ionomer interface through an accelerated stress test combined with electrochemical impedance spectroscopy. Various interfaces are created through catalyst inks prepared using commercial Pt/C catalyst powder dispersed in different solvents. Electrode degradation pattern turns out to be a very useful tool to interpret a catalyst/ionomer interface structure. Variations of interfacial impedance, electrochemical surface area (ECSA), and double layer capacitance with the number of potential cycles suggested significant impact of catalyst/ionomer interface on the catalyst performance. A quantification of the degradation mechanisms responsible for ECSA loss during AST was employed to further understand the correlations between the electrochemical performance of the electrodes and their catalyst/ionomer interface structures. The knowledge may be implied to further optimize the electrode structure and hence to advance the PEMFC technology.
聚合物电解质膜燃料电池(PEMFC)的大规模应用主要受到电极高初始成本和耐久性问题的限制,电极主要由纳米颗粒催化剂(如Pt)组成,这些催化剂分别通过催化剂载体、聚合物电解质离聚物和多孔气体扩散层与电子(e)、质子(H)以及燃料/氧化剂接触。因此,为了在活性和/或耐久性方面实现高电极性能,理解和优化催化剂/载体以及催化剂/离聚物界面至关重要。本研究展示了一种通过加速应力测试结合电化学阻抗谱来检测催化剂/离聚物界面的替代方法。通过使用分散在不同溶剂中的商业Pt/C催化剂粉末制备的催化剂墨水创建各种界面。电极降解模式被证明是解释催化剂/离聚物界面结构的非常有用的工具。界面阻抗、电化学表面积(ECSA)和双层电容随电位循环次数的变化表明催化剂/离聚物界面对催化剂性能有显著影响。对加速应力测试期间导致ECSA损失的降解机制进行量化,以进一步了解电极的电化学性能与其催化剂/离聚物界面结构之间的相关性。这些知识可能有助于进一步优化电极结构,从而推动PEMFC技术的发展。