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

J Colloid Interface Sci. 2021 Aug 15:596:12-21. doi: 10.1016/j.jcis.2021.03.116. Epub 2021 Mar 24.

Abstract

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 ~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 (~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.

Keywords: Charge imbalance; Hydrogen evolution; Mesoporous TiO(2); Photocatalysis; Surface defect.