Advances in the theoretical understanding of interfacial electrochemistry have, over the past decade, permitted the extension of periodic Density Functional Theory studies, which have traditionally been applied to probe chemistry at gas/solid interfaces, to electrochemical systems where potential-dependent structural and chemical phase transformations occur at liquid/solid interfaces. Indeed, such techniques have been employed to study a surprisingly wide class of electrochemical processes, ranging from electrocatalysis to corrosion, and are now being used to identify promising candidates for new electrocatalytic materials.

In this talk, I will provide a brief overview of current approaches to computational screening of electrocatalysts, focusing in particular on the need to couple predictions of catalyst stability with traditional analyses of rates and activities. I will begin with a discussion of recent results in the computational screening of oxygen reduction (ORR) electrocatalysts, focusing on the large number of materials “tuning knobs” that have been explored via calculations for this chemistry. I will then describe very recent efforts to computationally probe catalytic properties of more structurally complex electrocatalysts, including bifunctional catalysts and mixed metal/oxide systems. For such catalysts, which are relevant for chemistries ranging from CO oxidation in acidic solutions to hydrogen evolution in alkaline solutions, prediction of materials structure and stability is an essential prerequisite to determination of rates and currents, and I will therefore focus on how techniques to effect stability predictions are being combined with traditional screening methods for these systems. I will close with a few perspectives on future directions for electrocatalyst screening efforts.