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

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.