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In-situ generated hydrogen pump boosting photocatalytic hydrogen evolution over ZnCdS/MoO3-x under visible light irradiation

Wen Liao,Fangxia Xie,Lulu Zhang,Qing Xi,Long Cao,Yawen Wang,Yunfang Wang,Houfen Li,Rui Li,Caimei Fan,Jianxin Liu,Jiancheng Wang

Photocatalytic water splitting for hydrogen evolution (PHE) is an effective and sustainable strategy to alleviate energy shortages and environmental issues. However, active hydrogen (H*), as a critical intermediate, has low generation and desorption rates that limit the development of PHE. Herein, a ZnCdS/MoO 3-x heterojunction is prepared by a two-step solvothermal method and applied to a photocatalytic hydrogen evolution reaction under visible light conditions. The band structure and electron spin resonance (ESR) confirm the formation of an S-scheme heterojunction in ZnCdS/MoO 3-x , promoting the utilization of photo-generated carriers and thereby enhancing H* generation on ZnCdS. Furthermore, in-situ ESR, quasi in-situ Raman spectroscopy and in-situ DRFTIRS spectroscopy demonstrate that the H* is subsequently transferred from ZnCdS to MoO 3-x via the hydrogen spillover effect. The H* is then confined within the lattice of MoO 3-x and forms H x MoO 3-x in situ. Finally, the electrochemical tests and DFT calculations demonstrate that the H x MoO 3-x acts as a “hydrogen pump”, lowering the H* desorption barriers and ultimately enhancing the hydrogen evolution of the system. Therefore, the optimum hydrogen evolution rate of ZnCdS/MoO 3-x reaches 7.9 mmol·g −1 ·h −1 , which is 26.3 times higher than that of pure ZnCdS, along with a hydrogen storage capacity of 0.36 wt%. This work offers a novel approach for achieving efficient and sustained PHE reactions by modulating the generation and desorption rates of the intermediate H*.