(465e) Solvation Effects in Surface Electrochemistry for Oxygen Evolution Reaction Catalysis on Transition Metal Oxides
The Oxygen Evolution Reaction (OER) takes place at the anode of electrolytic water splitting. Currently, there are no good catalysts for the OER, regardless of pH . Many current ab-initio calculations for OER do not contain an explicit solvent , which has been shown to be significant for titanium dioxide [3,4], and for some other oxide surfaces . It is necessary to understand how water impacts the stability of surface-bound OER intermediates to better design and understand electrocatalysts.
In this work we use DFT calculations and a minima hopping global optimization method to investigate how the inclusion of explicit solvent molecules affects the binding energies of OER intermediates at various intermediate coverages. Our results on IrO2 indicate that hydrogen containing intermediates (*OH, *OOH) are significantly stabilized relative to O* by the explicit solvent. Relative stabilization of particular intermediates leads to changes in reaction energetics and ultimately in the calculation of theoretical overpotential, which is a measure of a catalystsâ?? activity . Furthermore, solvent interaction with adsorbed intermediates has potential to be important for other electrochemical reactions, such as N2 and CO2 reduction. As such, an understanding of these solvent interactions could greatly impact how we think about catalyst design.
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