Surface-induced strategy: Phosphorus-induced NiFe-LDH generation of strong surface bonding states for efficient photocatalytic hydrogen evolution

Light-driven semiconductor splitting of water for hydrogen production is becoming increasingly important in the direction of obtaining clean energy. In this study, high-temperature P-induced corrosion of NiFe-LDH was used to generate P-metal strong surface bonding states. The surface layout of Ni/Fe-P(δ−) covalent bonds on the one hand enriches the active sites for photocatalytic hydrogen evolution and opens up the valve for accelerated hydrogen production. On the other hand, it opens the migration channel for photogenerated electrons, which broadens the electron supply for photocatalytic hydrogen generation. FTIR spectroscopy and XPS results showed that Ni/Fe-P covalent bonds were successfully deployed on the catalysts. PL results showed that the introduction of covalent bonds had a facilitating effect on promoting the separation and migration of photogenerated electrons. The design of Ni-P(δ−) and Fe-P(δ−) bonds was further confirmed by In situ irradiated X-ray Photoelectron Spectroscopy to open the channels for trapping and transporting electrons. Based on the experimental results, we propose a possible bimolecular mechanism for synergistic hydrogen evolution, which provides novel and unique insights into the in-depth analysis of the influence of surface bonding states on the photocatalytic mechanism.