Enhancing photocatalytic H2O2 production with Au co-catalysts through electronic structure modification
Xidong Zhang, Duoduo Gao, Bicheng Zhu, Bei Cheng, Jiaguo Yu, Huogen Yu
Abstract
Abstract Gold-based co-catalysts are a promising class of materials with potential applications in photocatalytic H 2 O 2 production. However, current approaches with Au co-catalysts show limited H 2 O 2 production due to intrinsically weak O 2 adsorption at the Au site. We report an approach to strengthen O 2 adsorption at Au sites, and to improve H 2 O 2 production, through the formation of electron-deficient Au δ+ sites by modifying the electronic structure. In this case, we report the synthesis of TiO 2 /MoS x -Au, following selective deposition of Au onto a MoS x surface which is then further anchored onto TiO 2 . We further show that the catalyst achieves a significantly increased H 2 O 2 production rate of 30.44 mmol g −1 h −1 in O 2 -saturated solution containing ethanol. Density functional theory calculations and X-ray photoelectron spectroscopy analysis reveal that the MoS x mediator induces the formation of electron-deficient Au δ+ sites thereby decreasing the antibonding-orbital occupancy of Au-O ads and subsequently enhancing O 2 adsorption. This strategy may be useful for rationally designing the electronic structure of catalyst surfaces to facilitate artificial photosynthesis.