Optimizing Electronic Density at Active W Sites for Boosting Photocatalytic H 2 Evolution

作者：Jing Xu, Xueqi Zhang, Wei Yan, Tengfeng Xie, Yuanping Chen, Yingcong Wei · 发表于：Inorganic Chemistry · 年份：2024 · DOI：10.1021/acs.inorgchem.3c04408 · 被引用次数：27 · 研究领域：Advanced Photocatalysis Techniques、Gas Sensing Nanomaterials and Sensors、ZnO doping and properties

It is highly desirable but challenging to optimize the electronic structure of an active site to realize moderate active site-H ads bond energies for boosting photocatalytic H 2 evolution. Herein, an interfacial engineering strategy is developed to simultaneously concentrate hydrogen species and accelerate the combination of an H ads intermediate to generate free H 2 by constructing W–WC–W 2 C (WCC) cocatalysts. Systematic investigations reveal that hybridizing with W 2 C creates electron-rich W active sites and effectively induces the downshift of the d-band center of W in WC. Consequently, the strong W–H ads bonds on the surface of WC are weakened, thus promoting the desorption of H ads to rapidly produce free H 2 . The optimized 40-WCC/CdS photocatalyst exhibits a high hydrogen evolution rate of 63.6 mmol g –1 h –1 under visible light (≥420 nm) with an apparent quantum efficiency of 39.5% at 425 nm monochromatic light, which is about 40-fold of the pristine CdS. This work offers insights into the design of cocatalyst for high-efficiency photocatalytic H 2 production.