Piezoceramics Boosting Photocatalytic Hydrogen Evolution of Covalent Organic Frameworks

Abstract Precise manipulation of charge‐carrier transport dynamics is a pivotal yet challenging attribute in enhancing the efficiency of energy‐conversion systems. Herein, piezopotential and optimized energy band alignment are leveraged to construct a core–shell Z ‐scheme heterostructure, covalently bonding BaTiO 3 nanowires (a piezoelectric ceramic) with TpPa (an imine‐linked covalent organic framework). This synergistic combination effectively overcomes the intrinsic limitations of the individual components, particularly in driving photocatalytic water splitting. The resultant Z ‐scheme heterostructure exhibits a broadened visible‐light absorption range, finely tuned energy band alignment, abundant exposure of active sites, and enhanced piezo‐driven charge separation, collectively leading to remarkable improvements in charge‐carrier transfer and utilization efficiency. As a result, an impressive H 2 evolution rate of 33 mmol g −1 h −1 and an outstanding apparent quantum yield of 9.39% are achieved, representing enhancements of 4.56‐fold and 10.06‐fold, respectively, compared to pure photocatalysis. This work presents an effective strategy for designing high‐efficiency catalysts and highlights the potential of piezoelectricity in boosting photo‐redox reactions.