Promoting Photocatalytic H₂ Evolution through Retarded Charge Trapping and Recombination by Continuously Distributed...

Inspired by its great success in the photovoltaic field, methylammonium lead iodide perovskite (MAPbI₃ ) has recently been actively explored as photocatalysts in H₂ evolution reactions. However, the practical application of MAPbI₃ photocatalysts remains hampered by the intrinsically fast trapping and recombination of photogenerated charges. Herein, we propose a novel strategy of regulating the distribution of defective areas to promote charge-transfer dynamics of MAPbI₃ photocatalysts. By deliberately designing and synthesizing the MAPbI₃ photocatalysts featuring a unique continuation of defective areas, we demonstrate that such a feature enables retardation of charge trapping and recombination via lengthening the charge-transfer distance. As an outcome, such MAPbI₃ photocatalysts turn out to achieve an impressive photocatalytic H₂ evolution rate as high as 0.64 mmol ⋅ g^-1  ⋅ h^-1 , one order of magnitude higher than that of the conventional MAPbI₃ photocatalysts. This work establishes a new paradigm for controlling charge-transfer dynamics in photocatalysis.