Stabilizing electron-rich Ni single-atoms on black phosphorus nanosheets boosts photocatalytic carbon dioxide reduction

J Colloid Interface Sci. 2024 Mar 15:658:324-333. doi: 10.1016/j.jcis.2023.12.075. Epub 2023 Dec 13.

Abstract

The development of unique single-atom catalysts with electron-rich feature is essential to promoting the photocatalytic CO2 reduction, yet remains a big challenge. Here, a conceptionally new single-atom catalyst constructed from atomically dispersed Ni-P3 species on black phosphorus (BP) nanosheets (BP-Ni) is synthesized for realizing highly efficient visible-light-driven CO2 reduction when trapping photogenerated electrons from homogeneous light absorbers in the presence of triethanolamine as the sacrificial agent. Both the experimental and theoretical calculation data reveal that the Ni-P3 species on BP nanosheets own the electron-rich feature that can improve the photogenerated charge separation efficiency and lower the activation barrier of CO2 conversion. This unique feature makes BP-Ni exhibit the much higher activity as cocatalyst in the photocatalytic CO2 reduction than BP nanosheets. The BP-Ni can also be applied as a cocatalyst for enhanced photocatalytic CO2 reduction after combining with CdSe/S colloidal crystal photocatalyst. The present study offers valuable inspirations for the design and construction of effective catalytic sites toward photocatalytic CO2 reduction reactions.

Keywords: Black phosphorus; Cocatalyst; Photocatalytic CO(2) reduction; Single-atom catalyst.