Pt single-atom loaded on nonmetallic elements (C, N, P, S) doped ZrO2 in photocatalytic hydrogen evolution: First principles

Abstract

It is of great significance to regulate the coordination environment of ZrO2 to enhance its photocatalytic hydrogen evolution activity. In this paper, non-metallic elements (A = C, N, P, S) doped ZrO2 photocatalysts are designed based on first-principles, and further loaded with single-atom Pt. The relationship between the composition and performance of photocatalysts during doping and loading of single-atom is explained through electronic properties, and their photocatalytic hydrogen evolution performance is explored. Loading and doping have a synergistic effect on the modification of ZrO2, and doping effectively improves its catalytic performance. Among them, P doping greatly reduces the Gibbs free energy of the reaction. After the introduction of Pt single atoms, Pt@ZrO2(111)-P still has the best structure for photocatalytic hydrogen evolution, and the good surface electronic activity significantly improves the hydrogen evolution reaction(HER) activity (free energy of −0.01 eV). This design provides a new catalytic model for the photocatalytic hydrogen evolution system and also provides some ideas for understanding the synergistic effects of loading and doping.

Keywords

• First principles
• Single-atom catalyst
• Coordination environment
• Photocatalysis
• Hydrogen evolution reaction