Synergistic surface oxygen defect and bulk Ti3+ defect engineering on SrTiO3 for enhancing photocatalytic overall water splitting

SrTiO3 as a photocatalytic overall water splitting material has received extensive attention in recent years, while effectively suppressing Ti3+ is the key to enhancing the photocatalytic performance. Herein, a polymerizable complexation method is employed to enable Al3+ uniformly enter into SrTiO3 lattice for reducing Ti3+, and substituting Ti4+ with the formation of oxygen vacancy. Thus, the photogenerated carrier transport is promoted, and the resulting appropriate surface oxygen vacancy is also conducive to the adsorption of water molecules and OH*. The optimized 2% Al3+-doped SrTiO3 possesses a lower Ti3+ concentration, compared with the same sample prepared by the solid-phase griding method. Consequently, 2% Al-STO sample deposited co-catalysts achieves the highest activity and durability with the H-2 and O-2 evolution rates of 1.256 mmol.h(-1) and 0.692 mmol.h(-1) (0.04 g catalyst), respectively, corresponding to the AQE value of 55.46% at 365 nm. The characterizations and DFT calculation results reveal that the uniform Al3+ doping promotes the increase in the surface oxygen vacancy, which is beneficial for accelerating the reduction reaction and facilitating carrier separation and migration, therefore enhancing the overall water splitting reaction. (C) 2022 Published by Elsevier Inc.

Automated summary

In this study, a polymerizable complexation method was used to uniformly introduce Al3+ into the lattice of SrTiO3, reducing the concentration of Ti3+ and creating oxygen vacancies. This promoted the transport of photogenerated carriers and facilitated the adsorption of water molecules and OH*. The optimized 2% Al3+-doped SrTiO3 exhibited the highest catalytic activity and durability.