Proceedings of Materials for Sustainable Development Conference (MAT-SUS) (NFM22)
DOI: https://doi.org/10.29363/nanoge.nfm.2022.277
Publication date: 11th July 2022
Once solar fuels are accessible economically and widely, we need a device to convert them into useful energy. In this aspect, fuel cells (FCs) are more appealing than conventional internal combustion engine in terms of energy efficiency because of no entropy energy waste. However, mass deployment of FCs demands better electrode-electrolyte interfaces to catalyze oxygen reduction reaction (ORR, especially in acidic environments), the kinetics of which depends on the energetics of surface adsorption as well as on the electrolyte environment. While the former has been well established using experimental and theoretical work, the effect of the electrolyte remains relatively unexplored. In this talk, I will first show an unanticipated effect of nonspecifically adsorbing (NSA) anions on the ORR kinetics on a Pt(111) electrode in acid. The electrolyte-related trends do not follow the usual ORR descriptor, i.e. *OH binding energy. Instead, a new voltammetry-accessible descriptor, namely the reversibility of the *O↔*OH transition on the (111) terrace was proposed to successfully track the dependence of ORR rates on electrolyte properties, including the concentration/identity of NSA anions in acidic media, cations in alkaline media, and the effect of the presence of ionomers, as observed in this study and in the literature. An enhanced model that relates the ORR rate on Pt(111) to the rate of the *O to *OH transition, in addition to the traditional “thermodynamic” *OH binding energy descriptor, was established, suggesting that there is more than one descriptor for the overall ORR rate. Our updated picture of the ORR can help in rationalizing the different trends for the ORR rate on stepped Pt surfaces in acidic vs. alkaline media. This study paves an avenue towards a more complete understanding of the various factors that determine the ORR rate on Pt surfaces.
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