The problem of global warming has been known for decades and is believed to be linked directly to the exhaust of carbon dioxide and other gases into the atmosphere which are produced in the combustion of fossil fuel. Carbon-neutral energy sources can be obtained by converting abundant sunlight into chemical compounds. Prominent examples for reactions generating solar-fuel are the photo-electrochemically driven water splitting reaction and the carbon dioxide reduction at metal-oxide solid photo-catalysts.<br/>A detailed analysis of the involved elementary processes via first-principles calculations is challenging due to the necessity to simultaneously account for the extended semiconductor surface and the liquid electrolyte. Going beyond traditionally assumed proton-coupled electron transfer mechanisms one may furthermore face charged intermediate states where a significant stabilization due to the polar liquid environment is to be expected. This necessitates a method able to capture electrostatic solvent effects whilst being computationally inexpensive in order to allow for efficient catalyst screening. To this end, we implemented an implicit solvation scheme based on the multipole expansion method into the density functional theory package FHI-aims and discuss first investigations on the photo-electrocatalytic oxygen evolution reaction on rutile titanium dioxide surfaces.

Continuum embedding for photo-electrochemical surface processes

251st National Meeting (2016)

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