Remarkably Enhanced Hydrogen Generation of Organolead Halide Perovskites via Piezocatalysis and Photocatalysis

To alleviate photoinduced charge recombination in semiconducting nanomaterials represents an important endeavor toward high‐efficiency photocatalysis. Here a judicious integration of piezoelectric and photocatalytic properties of organolead halide perovskite CH 3 NH 3 PbI 3 (MAPbI 3 ) to enable a piezophotocatalytic activity under simultaneous ultrasonication and visible light illumination for markedly enhanced photocatalytic hydrogen generation of MAPbI 3 is reported. The conduction band minimum of MAPbI 3 is higher than hydrogen generation potential (0.046 V vs normal hydrogen electrode), thereby rendering efficient hydrogen evolution. In addition, the noncentrosymmetric crystal structure of MAPbI 3 enables its piezoelectric properties. Thus, MAPbI 3 readily responds to external mechanical force, creating a built‐in electric field for collective piezophotocatalysis as a result of effective separation of photogenerated charge carriers. The experimental results show that MAPbI 3 powders exhibit superior piezophotocatalytic hydrogen generation rate (23.30 µmol h −1 ) in hydroiodic acid (HI) solution upon concurrent light and mechanical stimulations, much higher than that of piezocatalytic (i.e., 2.21 µmol h −1 ) and photocatalytic (i.e., 3.42 µmol h −1 ) hydrogen evolution rate as well as their sum (i.e., 5.63 µmol h −1 ). The piezophotocatalytic strategy provides a new way to control the recombination of photoinduced charge carriers by cooperatively capitalizing on piezocatalysis and photocatalysis of organolead halide perovskites to yield highly efficient piezophotocatalysis.