First-principles calculations combining density-functional theory (DFT) and continuum solvation models have been highly successful in enabling the theoretical design of liquid-phase catalyst materials. The application of such methods to heterogeneous catalysis in electrochemical solid-liquid interfaces has however been far more challenging for two reasons. First, conventional continuum solvation methods designed for finite molecular systems are not readily applicable to solid-liquid interfaces with metal or oxide surfaces. Second, processes at these interfaces continuously exchange electrons with the electrode, which makes the charge states of the surface difficult to determine.<br/><br/>I will present recent developments in continuum solvation methods that enable accurate treatment of solid surfaces and molecules in electrochemical interfaces. Additionally, by automatically equilibrating charge at a fixed electrochemical potential, new 'grand-canonical DFT' algorithms and software (JDFTx) facilitate realistic description of processes in these interfaces. I will provide a brief overview of applications of these methods to electro- and photo-catalysis for energy conversion, and to battery materials. I will end with an outline of pending challenges and future developments for first-principles electrochemistry.

First-principles methods for modeling electrochemical processes

254th National Meeting (2017)

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