Integrating electronic structure regulation and dynamic active sites construction on NixCd1-xS-Ni0 photocatalyst for efficient hydrogen

Regulating electronic structure and enriching active sites of photocatalysts are effective strategies to promote hydrogen evolution. Herein, a unique NixCd1-xS-Ni-0 photocatalyst, including the surface nickel (Ni) doping and atomic Ni0 anchoring sites, is successfully prepared by Ni2+ ions exchange reaction (Ni2+ + CdS -> NixCd(1-x)S) and in-situ photo-induction of Ni-0 (Ni2+ + NixCd1-xS ->(NiCd1-xS)-Ni-h nu-Cd-x - Ni-0), respectively. As to Ni doping, the Ni replaced cadmium (Cd) atoms introduce hybridized states around the Fermi level, modulating the electronic structure of adjacent S atoms and optimizing the photocatalytic activity of sulfur (S) atoms. Besides, photogenerated Ni-0 atoms, anchored on unsaturated S atoms, act as charge transfer bridges to reduce Ni2+ ions in the solution to Ni clusters (NixCd1-xS - Ni (2H+)-> H2 up arrow NixCd1-xS-Ni-0). Subsequently, the displacement reaction of Ni clusters with protons (H+) spontaneously proceeds to produce hydrogen (H2) in an acidic solution (Ni(x)Cd1-xS - Ni (2H+) -> H2 up arrow +Ni2+ NixCd1-xS- Ni-0 ). The equilibrium of photo-deposition/dissolution of Ni clusters realizes the construction of dynamic active sites, providing sustainable reaction centers and enhancing surface redox kinetics. The NixCd1-xS-Ni-0 exhibits

Automated summary

Regulating the electronic structure and enriching active sites of photocatalysts are effective strategies to promote hydrogen evolution. In this study, a unique NixCd1-xS-Ni-0 photocatalyst with surface Ni doping and atomic Ni0 anchoring sites was successfully prepared. Ni doping modulates the electronic structure of adjacent S atoms, while anchored Ni-0 atoms facilitate the production of hydrogen. The NixCd1-xS-Ni-0 photocatalyst exhibits excellent photocatalytic performance.