Efficient charge separation in sulfur doped AgFeO2 photocatalyst for enhanced photocatalytic U(VI) reduction: The role of doping and mechanism insights

Photocatalytic reduction of U(VI) in aqueous solutions has been considered as an efficient and promising technology to solve radioactive U pollution. In this work, density functional theory (DFT) calculations were firstly employed to optimize and compare the adsorption configurations combined uranium with four given photocatalysts, then their adsorption energies were -0.97 eV for AgFeO2, -1.15 eV for Zn doped AgFeO2, -1.73 eV for Cu doped AgFeO2 and -2.66 eV for S doped AgFeO2, respectively, indicating the sulfur doping plays a major role in U(VI) photoreduction. Herein, a visible light responsive efficient sulfur doped AgFeO2 photo -catalyst (S doped AgFeO2) was synthesized and utilized to photocatalytic reduction of U(VI) in aqueous solutions. According to XRD, XPS and TEM analysis, the sulfur was successfully doped in AgFeO2 via the hydrothermal method. The batch experimental showed that S doping enhanced the U(VI) photoreduction activity of AgFeO2, and the S-AFO-3 photocatalyst exhibited the highest photocatalytic activity (92.57%), which was 1.5 times than that of pure AgFeO2. ESR, PL and DFT results demonstrated that the enhancement of adsorbed U(VI) photoreduction was attributed to the own unique effect of oxygen vacancy defects and efficient charge separation of S doped AgFeO2 photocatalyst. Due to its higher adsorption energies, fast-U(VI) photoreduction rate and superior chemical stability, the sulfur doped AgFeO2 photocatalyst is hoped for water remediation containing U(VI) wastewater.