Function-oriented design of robust metal cocatalyst for photocatalytic hydrogen evolution on metal/titania composites

Abstract While the precise design of catalysts is one ultimate goals in catalysis, practical strategies often fall short, especially for complicated photocatalytic processes. Here, taking hydrogen evolution reaction (HER) as an example, we introduce a theoretical approach designing robust metal cocatalysts supported on TiO 2 using density functional theory calculations adopting on-site Coulomb correction and/or hybrid functionals. The starts with clarifying individual function each layer metal/TiO composites HER, covering both electron transfer and surface catalysis aspects, followed by conducting function-oriented optimization via exploring competent candidates. With this approach, successfully determine verify bimetallic Pt/Rh/TiO Pt/Cu/TiO to be substitutes conventional Pt/TiO . right type well proper stacking sequence are demonstrated key boosting performance. Moreover, tentatively identify tunneling barrier height effective descriptor important process photocatalysis metal/oxide catalysts. We believe that study pushes forward frontier photocatalyst towards higher water splitting efficiency.