KSCN-activation of hydrogenated NiO/TiO_2 for enhanced photocatalytic hydrogen evolution

摘要

It was investigated the efficiency of hydrogen production from NiO-loaded TiO2 treated by methanol hydrogenation and functionalized by SCN ligand (SCN-M:(NiO/TiO2)). The effects of a p-n junction created between NiO and TiO2 were demonstrated to enhance significantly the overall photocatalytic performance. The optical and microstructural properties of SCN-M:(NiO/TiO2) were studied with ultraviolet-visible spectra (UV-Vis), photoluminescence (PL), Raman spectra, X-ray diffraction (XRD) and X-ray photoelectron spectra (XPS). The atomic and electronic configurations of SCN-M:(NiO/TiO2) were investigated with analysis of the X-ray absorption near-edge structure (XAS) in situ under irradiation with Xe lamp incorporating a filter (AM 1.5G). An effective quantum yield of 1.34% for hydrogen production was attained with SCN-M:(NiO/TiO2). Quantum-chemical calculations revealed a synergistic decrease of the band gap upon loading Ni, Ni-linked O-2 and anionic SCN-ligand binding. The optimal energy bandgap was decreased to 2.70 eV for (SCN/O-2)-3Ni@TiO2, which reasonably supported the enhancement of H-2 evolution.