揭示 Zn_xCd_1-xS 固溶体光催化析氢中的直接-间接带隙跃迁机制

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关键词： ZnxCdl-xS 固溶体；光催化析氢；光生载流子转移；直接-间接带隙跃迁

中图分类号：0643

doi： 10.1016/j.actphy.2025.100141

Unveiling the mechanism of direct-to-indirect bandgap transition in the photocatalytic hydrogen evolution of Zncd1-xS solid solution

Huoshuai Huang‘1， Zhidong Wei1.2*， Jiawei Yan 1，Jiasheng Chi 1， Qianxiang Su1，Mingxia Chen‘1， Zhi Jiang1 Yangzhou Sun ³， Wenfeng Shangguan 1.*

1 Research Center for Combustion and Environment Technology， Shanghai Jiao Tong University， Shanghai 200240， China.

2College of Smart Energy， Shanghai Jiao Tong University， Shanghai 20o240，China.

3 CNOOC Energy Economics Institute， Beijing 10013， China.

Abstract：Solid solution strategy could improve the photocatalytic performance thermodynamicaly，yet the study focusing on the carrier dynamics of the solid solution catalysts was equally important. Herein，a series of ZnxCd1-xS （2号 solid solutions were successfullysynthesized based onband 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 ZnxCd1-xS solid solution. The indirect bandgap exhibited alower photocarierrecombinationrate and，more importantly，couldalsoserveasatrappingcenter forphotocarier， thus promoting the efficiency of charge separation. Consequently， ZnxCd1-xS solid solutions achieved an approximately eleven-fold enhancement in the hydrogen evolution rate ）relative to that of bare Cds （ 129.83μmolh-1 ）undervisiblelight （>420nm） . 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.

Key Words： ZnxCd1-xS solid solution;Photocatalytic hydrogen evolution;Photocarrier transfer; Direct-to-Indirect transition

1引言

作为绿色能源转换的重要方向，光催化析氢（PHE）技术受到了广泛关注[1-4]。（剩余18673字）