Surface defects induced charge imbalance for boosting charge separation and solar-driven photocatalytic hydrogen evolution

Low charge separation efficiency of semiconductor materials is the main obstacle for high-performance photocatalyst. Herein, we report surface defects engineered uniform mesoporous TiO 2 nanospheres (DMTNSs) through surfactant-mediated self-assembly solvothermal approach combined with hydrogenation strategy to promote charge separation. The surface defects induced charge imbalance result in the formation of built-in field, which can promote photogenerated charge separation efficiently and be confirmed by experimental and density functional theory (DFT) calculations. Under AM 1.5G irradiation, the photocatalytic hydrogen evolution of DMTNSs is ~3.34 mmol h −1 g −1 , almost 3.5 times higher than that of pristine non-defective TiO 2 nanospheres (0.97 mmol h −1 g −1 ), due to the engineered surface defects narrowing the bandgap (~3.01 eV) and inducing charge imbalance to boost spatial charge separation and extend visible-light response. The defect induced charge imbalance strategy opens a new valuable perspective for fabricating other high-efficient oxide photocatalysts.