Unveiling Intrinsic Charge Transfer Dynamics in Bone-Joint S-Scheme Heterostructures To Promote Photocatalytic Hydrogen Peroxide Generation

Constructing compact direct Z- and S-scheme heterostructures is an efficient strategy for realizing a highly efficient charge separation and photocatalytic performance. However, the stochastic nature of interface orientation and lattice mismatch often results in a blind region for effective inner charge transfer, which hinders the logical design of compact heterojunctions. Here, experimental results and theoretical research unveiled that complicated internal charges can be directly transferred to an intermediate cocrystal plane for electron–hole recombination in compact S-scheme heterostructures, called “bone-joint” heterostructures, which facilitate the establishment of an inherent electric field to drive charge transfer. Moreover, those bone-joint structures adjust the inherent chemical and energetic interactions that manipulate the reactant adsorption mode and surface reaction energy. As a result, a synthesized catalyst displayed a remarkable hydrogen peroxide production performance and stability. This offers a paradigm for intrinsic charge transfer dynamics in heterostructures and a guiding philosophy for designing efficient heterostructures.