Embedding Nano‐Piezoelectrics into Heterointerfaces of S‐Scheme Heterojunctions for Boosting Photocatalysis and Piezophotocatalysis

Abstract Step‐scheme (S‐scheme) heterojunctions have exhibited great potential in photocatalysis due to their extraordinary light harvesting and high redox capacities. However, inadequate S‐scheme recombination of useless carriers in weak redox abilities increases the probability of their recombination with useful ones in strong redox capabilities. Herein, a versatile protocol is demonstrated to overcome this impediment based on the insertion of nano‐piezoelectrics into the heterointerfaces of S‐scheme heterojunctions. Under light excitation, the piezoelectric inserter promotes interfacial charge transfer and produces additional photocarriers to recombine with useless electrons and holes, ensuring a more thorough separation of powerful ones for CO 2 reduction and H 2 O oxidation. When introducing extra ultrasonic vibration, a piezoelectric polarization field is established, which allows efficient separation of charges generated by the embedded piezoelectrics and expedites their recombination with weak carriers, further increasing the number of strong ones participating in the redox reactions. Encouraged by the greatly improved charge utilization, significantly enhanced photocatalytic and piezophotocatalytic activities in CH 4 , CO, and O 2 production are achieved by the designed stacked catalyst. This work highlights the importance in strengthening the necessary charge recombination in S‐scheme heterojunctions and presents an efficient and novel strategy to synergize photocatalysis and piezocatalysis for renewable fuels and value‐added chemicals production.