Construction of a ZnS/ZnO@g-C3N4 Ternary Double Type-II Heterojunction for Enhanced Photocatalytic Hydrogen Evolution
摘要
ZnS/ZnO core-shell particles were synthesized via an in-situ displacement method and subsequently integrated with g-C3N4 through calcination to construct ZnS/ZnO@g-C3N4 ternary composites. The effects of the sulfidation degree and g-C3N4 coupling ratio on the morphology, optical absorption, charge-separation behavior, and photocatalytic H2-evolution performance were systematically investigated. Compared with pristine ZnO and binary ZnS/ZnO, the ternary composites exhibited markedly enhanced photocatalytic activity under visible-light irradiation. Among all samples, ZnS/ZnO@g-C3N4-1 showed the best performance, with a cumulative H2 production of about 295 μmol after 180 min and an actual H2 evolution rate of 98.50 μmol h-1 under identical reaction conditions, which is 3.28 times that of pristine ZnO. Photoelectrochemical measurements revealed improved charge separation and lower interfacial charge-transfer resistance in the optimized composite. XPS analysis further indicated strengthened interfacial electronic interaction and charge redistribution among ZnS, ZnO, and g-C3N4. Based on the estimated band-edge positions and the actual architecture of the composite, the ternary system can be reasonably described as a double type-II heterojunction, in which ZnS serves as the key interfacial bridge for charge transfer. In addition, the optimized photocatalyst maintained stable H2 production during cyclic tests, and post-reaction XPS results confirmed good chemical stability. This work provides a feasible strategy for constructing ZnO-based multicomponent heterojunction photocatalysts for photocatalytic hydrogen evolution.
Graphical Abstract