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Coupling impurity-state engineering with interfacial charge redis-tribution for efficient noble-metal-free photocatalytic hydrogen evolution
Hanmei Yang, Ping Zhou, Xinyu Xu, Bo Su, Xiahui Lin, Binbin Guo*, Xue Feng Lu, Kunlong Liu*, Guigang Zhang, Sibo Wang*
https://doi.org/10.1016/j.cjsc.2026.101101
Photocatalysis; Hydrogen evolution; Cd doping; Charge transfer; Impurity states
ABSTRACT
Photocatalytic hydrogen evolution is limited by inefficient charge separation and sluggish interfacial charge-transfer kinetics, necessitating the delicate modulation of carrier-transfer pathways to improve solar-to-hydrogen conversion efficiency. Herein, we report a noble-metal-free Cd-doped ZnS@ethylenediamine photocatalyst (Cd-ZnS@EDA) synthesized via a one-step solvothermal coordination-mediated self-assembly strategy. Cd incorporation generates impurity states within ZnS, which broaden excitation pathways, facilitate carrier redistribution, accelerate electron migration, and suppress charge recombination. Simultaneously, coordinated EDA constructs an amine-rich interface, promoting directional charge separation and interfacial electron migration. Moreover, the amine-rich interfacial environment is expected to facilitate proton adsorption near the catalyst surface and quickens proton-reduction kinetics. Benefiting from the coupling of impurity-state engineering and interfacial charge regulation, Cd-ZnS@EDA exhibits substantially improved charge generation, separation, transport, and utilization while effectively mitigating photocorrosion. As a result, the optimized catalyst affords an H2 evolution rate of 97.1 mmol g-1 h-1, outperforming both ZnS@EDA and Cd-ZnS, together with an apparent quantum efficiency of 30.6% and decent cycling stability. Combined experimental and theoretical investigations reveal that the cooperative effects of Cd-induced impurity states and EDA-mediated interfacial charge redistribution are responsible for the improved photocatalytic performance. This work establishes an effective strategy for integrating electronic-structure engineering with molecular interfacial regulation to develop efficient noble-metal-free photocatalysts for hydrogen production.
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CN 35–1112/TQ, ISSN 0254–5861, Online ISSN: 2949-768X Copyright @ 2022 Chinese Journal of Structural Chemistry-www.Chinese Journal of Structural Chemistry.net. All Rights Reserved 闽ICP备2022002645号-1