Citation: Huoshuai Huang, Zhidong Wei, Jiawei Yan, Jiasheng Chi, Qianxiang Su, Mingxia Chen, Zhi Jiang, Yangzhou Sun, Wenfeng Shangguan. Unveiling the mechanism of direct-to-indirect bandgap transition in the photocatalytic hydrogen evolution of Zn_xCd₁₋_xS solid solution[J]. Acta Physico-Chimica Sinica, ;2026, 42(1): 100141. doi: 10.1016/j.actphy.2025.100141 shu

Unveiling the mechanism of direct-to-indirect bandgap transition in the photocatalytic hydrogen evolution of Zn_xCd₁₋_xS solid solution

1.
Research Center for Combustion and Environment Technology, Shanghai Jiao Tong University, Shanghai 200240, China;
2.
College of Smart Energy, Shanghai Jiao Tong University, Shanghai 200240, China;
3.
CNOOC Energy Economics Institute, Beijing 100013, China

Corresponding author: Zhidong Wei, Wenfeng Shangguan,
Received Date: 16 June 2025
Revised Date: 24 July 2025

Solid solution strategy could improve the photocatalytic performance thermodynamically, yet the study focusing on the carrier dynamics of the solid solution catalysts was equally important. Herein, a series of Zn_xCd₁₋_xS solid solutions were successfully synthesized based on band structure regulation, and the carrier dynamics were investigated by femtosecond transient absorption spectroscopy (TAS) and DFT, which unveiled a variation of the mixed direct-to-indirect bandgap transition mechanism in Zn_xCd₁₋_xS solid solution. The indirect bandgap exhibited a lower photocarrier recombination rate and, more importantly, could also serve as a trapping center for photocarrier, thus promoting the efficiency of charge separation. Consequently, Zn_xCd₁₋_xS solid solutions achieved an approximately eleven-fold enhancement in the hydrogen evolution rate (1426.66 μmol h⁻¹) relative to that of bare CdS (129.83 μmol h⁻¹) under visible light (> 420 nm). This work proposed that the enhanced photocatalytic performance could originate from both thermodynamic and kinetic aspects simultaneously, and that the alteration of the photocarrier transition mechanism is one of the main factors affecting the kinetics.
- Zn_xCd₁₋_xS solid solution,
- Photocatalytic hydrogen evolution,
- Photocarrier transfer,
- Direct-to-Indirect transition,
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Unveiling the mechanism of direct-to-indirect bandgap transition in the photocatalytic hydrogen evolution of ZnxCd1−xS solid solution

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Unveiling the mechanism of direct-to-indirect bandgap transition in the photocatalytic hydrogen evolution of Zn_xCd₁₋_xS solid solution