Abstract
It is highly necessary but challenging to modify sulfides at the atomic scale to boost the separation of electron-hole pairs for enhanced photocatalytic performance. In this regard, single Rh atoms (Rh1) are assembled on CdZnS support with S vacancy defects (def-CZS) through RhS bond, creating a highly efficient photocatalyst. The optimized Rh1/def-CZS achieves an outstanding hydrogen evolution activity (30,512 μmol h−1 g−1), 4.32 and 3.34 folds enhancement that of CZS and def-CZS, respectively. The defective CZS support provides abundant S vacancy defects for Rh atom anchoring, where Rh bonds with neighboring S atoms (RhS). Theoretical calculations suggest that Rh can not only act as new H generation-release sites, but also optimize electron distribution around S defects simultaneously through the RhS bond, facilitating the separation of electron-hole pairs. Furthermore, in line with DFT results, in situ Raman confirms Rh (RhH) and electron-rich S atoms (SH) two main sites for proton reduction during hydrogen evolution.
Published Version
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