Quantifying Confidence in DFT-Predicted Surface Pourbaix Diagrams of Transition-Metal Electrode-Electrolyte Interfaces

Langmuir : the ACS Journal of Surfaces and Colloids
Olga VinogradovaVenkatasubramanian Viswanathan

Abstract

Density functional theory (DFT) calculations have been widely used to predict the activity of catalysts based on the free energies of reaction intermediates. The incorporation of the state of the catalyst surface under the electrochemical operating conditions while constructing the free-energy diagram is crucial, without which even trends in activity predictions could be imprecisely captured. Surface Pourbaix diagrams indicate the surface state as a function of the pH and the potential. In this work, we utilize error-estimation capabilities within the Bayesian ensemble error functional with van der Waals correlations exchange correlation functional as an ensemble approach to propagate the uncertainty associated with the adsorption energetics in the construction of Pourbaix diagrams. Within this approach, surface-transition phase boundaries are no longer sharp and are therefore associated with a finite width. We determine the surface phase diagram for several transition metals under reaction conditions and electrode potentials relevant for the oxygen reduction reaction. We observe that our surface phase predictions for most predominant species are in good agreement with cyclic voltammetry experiments and prior DFT studies. We us...Continue Reading

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