Abstract
The rational design of hierarchical heterojunction photocatalysts with efficient spatial charge separation remains an intense challenge in hydrogen generation from photocatalytic water splitting. Herein, a noble-metal-free MoS2/g-C3N4/ZnIn2S4 ternary heterostructure with a hierarchical flower-like architecture was developed by in situ growth of 3D flower-like ZnIn2S4 nanospheres on 2D MoS2 and 2D g-C3N4 nanosheets. Benefiting from the favorable 2D-2D-3D hierarchical heterojunction structure, the resultant MoS2/g-C3N4/ZnIn2S4 nanocomposite loaded with 3 wt% g-C3N4 and 1.5 wt% MoS2 displayed the optimal hydrogen evolution activity (6291 μmol g−1 h−1), which was a 6.96-fold and 2.54-fold enhancement compared to bare ZnIn2S4 and binary g-C3N4/ZnIn2S4, respectively. Structural characterizations reveal that the significantly boosted photoactivity is closely associated with the multichannel charge transfer among ZnIn2S4, MoS2, and g-C3N4 components with suitable band-edge alignments in the composites, where the photogenerated electrons migrate from g-C3N4 to ZnIn2S4 and MoS2 through the intimate heterojunction interfaces, thus enabling efficient electron-hole separation and high photoactivity for hydrogen evolution. In addition, the introduction of MoS2 nanosheets highly benefits the improved light-harvesting capacity and the reduced H2-evolution overpotential, further promoting the photocatalytic H2-evolution performance. Moreover, the MoS2/g-C3N4/ZnIn2S4 ternary heterostructure possesses prominent stability during the photoreaction process owing to the migration of photoinduced holes from ZnIn2S4 to g-C3N4, which is deemed to be central to practical applications in solar hydrogen production.
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