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Constructing spatially separated redox-active sites via atomically dispersed Ni doping on twinned Cd0.5Zn0.5S for efficient photocatalytic hydrogen evolution
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DOI：10.1016/j.jechem.2026.08.002.png)
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Abstract
En 中文
CdxZn1−xS-based photocatalysts hold tremendous potential for visible-light photocatalytic hydrogen production due to their unique solid solution structure and tunable band gap. However, their performance is typically constrained by insufficient active sites, sluggish electron transfer kinetics, and poor hydrogen adsorption/desorption capability. Cation doping can not only effectively increase the number of surface active sites but also promote the separation and transfer of photogenerated electrons by modulating the local electronic structure and coordination environment. Herein, this study reports an atomic-scale doping strategy, in which non-noble metal Ni is atomically dispersed into tetrahedral Zn sites within the hexagonal phase of twinned Cd0.5Zn0.5S (CZS). Without additional co-catalysts, the optimized Ni-CZS achieves a H2 evolution rate of 61.37 mmol g−1 h−1 and an apparent quantum efficiency (AQE) of 49.83% at 420 nm. Comprehensive characterizations and calculations confirm that the incorporation of Ni induces electron redistribution at twin interfaces, optimizing H* adsorption/desorption on S and Zn sites. Meanwhile, doped Ni serves as new oxidation-active sites, balancing redox kinetics and thus remarkably boosting the rate of the photocatalytic reaction. This work elucidates an atomic-scale Ni doping strategy to construct spatially separated redox active sites, providing a promising approach for designing efficient photocatalysts for solar hydrogen production.
Keywords:
Photocatalyst
Twin structures
Single atom doping
H2 evolution
CdxZn1−xS
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14.9
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4.5W
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