Publication date: 6th November 2020
Electrochemical CO2R is a particularly challenging process from both modelling and experimental perspectives. The challenge arises from the complexity of its reaction network and the sensitivity of its activity and selectivity to the electrolyte composition and the associated interfacial field effects. In this talk, I will first discuss developments in methods to model the electrochemical interface - the accuracy of widely applied continuum approximations of the electrolyte, as well as a new unified approach to obtain electrochemical barriers from both explicit and implicit solvent simulation approaches. In particular I emphasize that the surface charge gives the most appropriate proxy of the local potential (vs. the traditionally considered work function). Then, I will discuss the impact of the electrolyte composition - pH and ions - on electrochemical CO2R activity of both transition metals as well as supported single atom catalysts. Finally, I discuss the implications of our findings for electrocatalyst design and electrolyte engineering.
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