@article{35479, author = {ChungHyuk Lee and Xiaohua Wang and Jui-Kun Peng and Adlai Katzenberg and Rajesh K Ahluwalia and Ahmet Kusoglu and Siddharth Komini Babu and Jacob S Spendelow and Rangachary Mukundan and Rodney L Borup}, title = {Toward a Comprehensive Understanding of Cation Effects in Proton Exchange Membrane Fuel Cells}, abstract = {

Metal alloy catalysts (e.g., Pt–Co) are widely used in fuel cells for improving the oxygen reduction reaction kinetics. Despite the promise, the leaching of the alloying element contaminates the ionomer/membrane, leading to poor durability. However, the underlying mechanisms by which cation contamination affects fuel cell performance remain poorly understood. Here, we provide a comprehensive understanding of cation contamination effects through the controlled doping of electrodes. We couple electrochemical testing results with membrane conductivity/water uptake measurements and impedance modeling to pinpoint where and how the losses in performance occur. We identify that (1) ∼44% of Co2+ exchange of the ionomer can be tolerated in the electrode, (2) loss in performance is predominantly induced by O2 and proton transport losses, and (3) Co2+ preferentially resides in the electrode under wet operating conditions. Our results provide a first-of-its-kind mechanistic explanation for cation effects and inform strategies for mitigating these undesired effects when using alloy catalysts.

}, year = {2022}, journal = {ACS Applied Materials & Interfaces}, volume = {14}, pages = {35555 - 35568}, month = {08/2022}, issn = {1944-8244}, url = {https://pubs.acs.org/doi/10.1021/acsami.2c07085}, doi = {10.1021/acsami.2c07085}, language = {eng}, }