Elucidation of the Hydrogen Evolution Reaction on a Photochemical Molecular Device

Abstract One of the ultimate goals of photocatalysis is the direct utilzation of solar energy into the production of useful chemical products. In particular the direct photocatalytic water splitting to produce molecular hydrogen as a versatile, sustainable and ecologically friendly fuel is of great interest. This goal has motivated numerous research efforts to develop and improve corresponding photochemical molecular devices. However, it is fair to say that most of these efforts concentrated on the identification of the light-driven electron transfer processes within these devices, whereas the mechanistic details of the hydrogen evolution reaction remained largely unexplored. Here we present a first-principles based theoretical study of a photochemical molecular device that combines the determination of the light-driven electron transfer processes with the elucidation of the mechanistic details of the photo-induced hydrogen evolution reaction.