Interfacial Chemical Bond Engineering in a Direct Z-Scheme g-C₃N₄/MoS₂ Heterojunction

The Z-scheme heterojunction shows great potential in photocatalysis due to its superior carrier separation efficiency and strong photoredox properties. However, how to regulate the charge separation at the nanometric interface of heterostructures still remains a challenge. Here, we take g-C₃N₄ and MoS₂ as models and design the Mo-N chemical bond, which connects exactly the CB of MoS₂ and VB of g-C₃N₄. Thus, the Mo-N bond could act as an atomic-level interfacial “bridge” that provides a direct migration path of charge carriers between g-C₃N₄ and MoS₂. Experiments confirmed that the Mo-N bond and the internal electric field promote greatly the photogenerated carrier separation. The optimized photocatalyst exhibits a high hydrogen evolution rate that is about 19.6 times that of the pristine bulk C₃N₄. This study demonstrates the key role of an atomic-level interfacial chemical bond design in heterojunctions and provides a new idea for the design of efficient catalytic heterojunctions.