Intrinsically strained noble metal-free oxynitrides for solar photoreduction of CO2

Metal oxynitrides show promising activity for photocatalytic solar water splitting and CO2 reduction under solar irradiance. Precise control of cation ratios in oxynitrides is an inevitable challenge that needs to be overcome for achieving effective band gap tuning. Here we report the density functional theory-based calculations for the intricate structure-function relationships of Zn-Ga based oxynitrides and correlate the results with the experimental parameters. Crucial material property descriptors such as elemental composition, intrinsic lattice strain, and vacancy defects were exploited during the synthesis to achieve stable oxynitride photocatalysts that demonstrated CO2 conversion to CO under simulated solar light, without any noble metal impregnation. The highest CO production rate surpassed that of TiO2 under the same conditions. This work inspires future research on oxynitride materials with tailored optical properties and sustainable photocatalytic activity which enables their large scale applications.