title: First-principles thermodynamic screening approach to photo-catalytic water splitting with co-catalysts.
abstract: We adapt the computational hydrogen electrode approach to explicitly account for photo-generated charges and use it to computationally screen for viable catalyst/co-catalyst combinations for photo-catalytic water splitting. The hole energy necessary to thermodynamically drive the reaction is employed as descriptor for the screening process. Using this protocol and hybrid-level density-functional theory, we show that water oxidation on bare TiO2 surfaces is thermodynamically more complex than previously thought. This motivates a screening for suitable co-catalysts for this half-reaction, which we carry out for Au particles down to the non-scalable size regime. We find that almost all small Au clusters studied are better suited for water photo-oxidation than an extended Au(111) surface or bare TiO2 facets.
authors.affiliation: Department Chemie, Technische Universität München, Lichtenbergstr. 4, D-85747 Garching, Germany. harald.oberhofer@tum.de
authors.forename: Harald
authors.initials: H
authors.lastname: Oberhofer
authors.forename: Karsten
authors.initials: K
authors.lastname: Reuter