Two-dimensional Pd3(AsSe4)2 as a photocatalyst for the solar-driven oxygen evolution reaction: a first-principles study

The relationship between the structure and properties of materials is the core of material research. Bulk Pd-3(PS4)(2) materials have been successfully synthesized in the field of three-dimensional materials. After that, various studies on two-dimensional layered materials were conducted. Inspired by these successes, this work used density functional theory based on first principles to explore similar two-dimensional Pd-3(AsX4)(2), where X is S, Se, or Te belonging to the same group. Our findings demonstrate that the Pd-3(AsS4)(2) and Pd-3(AsSe4)(2) monolayers, with HSE06 band gaps of 2.37 and 1.36 eV, respectively, are indirect semiconductors. Additionally, their carrier mobilities [523.23 cm(2) s(-1) V-1 and 440.6 cm(2) s(-1) V-1] are also proved to be superior to MoS2 [similar to 200 cm(2) s(-1) V-1]. The optical calculations indicate that the Pd-3(AsSe4)(2) monolayer yields suitable valence band edge positions for the visible-light-driven water splitting reactions. More interestingly, at a low applied voltage of 0.14 V, Pd-3(AsSe4)(2) exhibits outstanding oxygen evolution reaction performance. In this study, the possible mechanism for the ability of Pd-3(AsSe4)(2) monolayer to promote photocatalysis and oxygen evolution was explained, which may pave the way for the practical design of further solar-driven high-quality water splitting photocatalysis.

Automated summary

The relationship between the structure and properties of materials is the core of material research. In this study, two-dimensional Pd-3(AsX4)(2) materials were explored using density functional theory based on first principles, and their properties as indirect semiconductors and their potential for photocatalysis and oxygen evolution were demonstrated.