| Summary: | Abstract In recent years, considerable research and development efforts are devoted to improving the performance of polymer electrolyte fuel cells. However, the power density and catalytic activities of these energy conversion devices are still far from being satisfactory for large-scale operation. Here we report performance enhancement via incorporation, in the cathode catalyst layers, of a ring-structured backbone matrix into ionomers. Electrochemical characterizations of single cells and microelectrodes reveal that high power density is obtained using an ionomer with high oxygen solubility. The high solubility allows oxygen to permeate the ionomer/catalyst interface and react with protons and electrons on the catalyst surfaces. Furthermore, characterizations of single cells and single-crystal surfaces reveal that the oxygen reduction reaction activity is enhanced owing to the mitigation of catalyst poisoning by sulfonate anion groups. Molecular dynamics simulations indicate that both the high permeation and poisoning mitigation are due to the suppression of densely layered folding of polymer backbones near the catalyst surfaces by the incorporated ring-structured matrix. These experimental and theoretical observations demonstrate that ionomer’s tailored molecular design promotes local oxygen transport and catalytic reactions.
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