Significantly Raised Visible‐Light Photocatalytic H 2 Evolution on a 2D/2D ReS 2 /In 2 ZnS 4 van der Waals Heterostructure

Owing to dwindling fossil fuels reserves, the development of alternative renewable energy sources is globally important. Photocatalytic hydrogen (H 2 ) evolution represents a practical and affordable alternative to convert sunlight into carbon‐free H 2 fuel. Recently, 2D/2D van der Waals heterostructures (vdWHs) have attracted significant research attention for photocatalysis. Here, for the first time a ReS 2 /In 2 ZnS 4 2D/2D vdWH synthesized via a facile physical mixing is reported. It exhibits a highly promoted photocatalytic H 2 ‐evolution rate of 2515 µmol h −1 g −1 . Importantly, this exceeds that for pristine In 2 ZnS 4 by about 22.66 times. This, therefore, makes ReS 2 /In 2 ZnS 4 one of the most efficient In 2 ZnS 4 ‐based photocatalysts without noble‐metal cocatalysts. Advanced characterizations and theoretical computations results show that interlayer electronic interaction within ReS 2 /In 2 ZnS 4 vdWH and atomic‐level S active centers along the edges of ReS 2 NSs work collaboratively to result in the boosted light‐induced H 2 evolution. Results will be of immediate benefit in the rational design and preparation of vdWHs for applications in catalysis/(opto)electronics.