Establishing Dual-Interface Built-In Electric Fields within Janus Heterostructures for Cooperative Photoredox Catalysis
Yi‐Wen Han, Yuxin Zhang, Lei Ye, Tian‐Jun Gong, Xuebin Lu, Ning Yan, Yao Fu
Abstract
Rationally designing nanostructures and comprehensively understanding the structure–property relationships are important for directional charge transfer. A general dual-interface built-in electric field (BIEF) regulation strategy is developed to synthesize the bifunctional ZnS/Sv-chalcogenide/Ti 3 C 2 heterostructure photocatalysts (Sv represents sulfur vacancies; chalcogenides include ZnIn 2 S 4, CdS, and CdIn 2 S 4 ) consisting of a ZnS/chalcogenide S-scheme heterojunction and a Sv-chalcogenide/Ti 3 C 2 Schottky heterojunction. The ternary-component photocatalyst construction involves hollow core–shell heterostructure establishment via lateral epitaxy and chalcogenide-surface Ti 3 C 2 nanoparticle introduction via a defect-mediated heterocomponent anchorage. These nanoreactors integrate the strong intrinsic driving force and enhanced interfacial electronic coupling, leveraging resulting dual-interface BIEFs for precise carrier mobility control and robust redox performance feedback. The BIEF-induced ultrafast charge transfer features powerful photocarrier enrichment and feeble photocarrier recombination at the ZnS/ZnIn 2 S 4 S-scheme heterointerface as well as continuous steering of photocarrier localization and delocalized electron transport at the Sv-ZnIn 2 S 4 /Ti 3 C 2 Schottky heterointerface. Simultaneously, BIEF-induced targeted molecule catalysis is marked by complementary adsorption and selective activation of key intermediates. Representative ZnS/Sv-ZnIn 2 S 4 /Ti 3 C 2 demonstrates broad substrate compatibility and superhigh reactivity in cooperative biomass valorization and hydrogen evolution. This study provides a programmable framework for manipulating BIEFs by multicomponent ordered-space integration and interface engineering, elucidating the substantial impact of dual-interface BIEFs on carrier transport behavior and molecular catalytic behavior.