Proceedings of nanoGe Fall Meeting19 (NFM19)
DOI: https://doi.org/10.29363/nanoge.nfm.2019.255
Publication date: 18th July 2019
Electrochemical CO2 reduction has been shown to be extremely sensitive to the composition of the electrolyte. In this talk I will discuss our theoretical investigations of 1) the effect of pH and 2) the effect of cation identity for CO2 reduction on Au, Ag, and Cu electrodes. Critical to both effects is the interfacial field- stabilization of relevant polar intermediates, which result in large shifts in activity with pH and ion identity. Based on ab initio simulations of reaction energetics and a modified Poisson Boltzmann approach to the ion distribution, we formulate corresponding kinetic models which are evaluated against experimental activity data. We discuss the implications of our findings for catalyst design and electrolyte engineering.
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