Juliana Cardoso Neves, Andrés Galdámez‐Martínez, Viktoriia Berezenko, Viktorija Pankratova, Yves Kayser, Taohai Li, Wei Cao
ZnIn 2 S 4 (ZIS) is a low-cost semiconductor with tunable morphology, suitable for visible-light water splitting, but limited by photocorrosion and low catalytic efficiency. To address these issues, we report an in-situ synthesis of ZIS/Ni-MOF-74 heterostructures, integrating 2D ZIS with Ni-MOF-74 to form a stable, efficient interface. This direct growth method preserves the MOF's structure and offers an alternative to post-synthetic assembly. The resulting composite achieves a hydrogen evolution rate five times higher than pristine ZIS and an apparent quantum efficiency (AQE) of 22,8 ± 1,2 % at 420 nm. Photocatalytic cycling confirms the material's stability. Spectroscopic analyses support an S-scheme charge transfer mechanism within the heterostructure. This work not only demonstrates a promising material for solar-driven hydrogen production and water purification but also encourages further exploration of sulfide-MOF combinations for broader photocatalytic applications. • In-situ growth of 2D ZnIn 2 S 4 /Ni-MOF heterostructures via controlled precipitation. • Mild synthesis conditions preserve Ni-MOF structure and functionality. • High HER of 2,33 mmol g −1 h −1 and 22,8 % AQE at 420 nm. • S-scheme mechanism supported by XAS and KPFM analysis.