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 TiO2 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 similar to 3.34 mmol h(-1) g(-1), almost 3.5 times higher than that of pristine non-defective TiO2 nanospheres (0.97 mmol h(-1) g(-1)), due to the engineered surface defects narrowing the bandgap (similar to 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. (C) 2021 Elsevier Inc. All rights reserved.