揭示ZnxCd1−xS固溶体光催化析氢中的直接-间接带隙跃迁机制

引用本文: 黄火帅, 韦之栋, 严嘉玮, 池家晟, 苏千翔, 陈铭夏, 江治, 孙洋洲, 上官文峰. 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[J]. 物理化学学报, 2026, 42(1): 100141. doi: 10.1016/j.actphy.2025.100141 shu

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_xCd_1−xS solid solution[J]. Acta Physico-Chimica Sinica, 2026, 42(1): 100141. doi: 10.1016/j.actphy.2025.100141 shu

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

黄火帅 ^1, ,
韦之栋 ^{1, 2,
,} ,
严嘉玮 ^1, ,
池家晟 ^1, ,
苏千翔 ^1, ,
陈铭夏 ^1, ,
江治 ^1, ,
孙洋洲 ^3, ,
上官文峰 ^{1,
,}

1.
上海交通大学燃烧与环境技术研究中心, 上海 200240
2.
上海交通大学智慧能源学院, 上海 200240
3.
中海油能源经济研究院, 北京 100013

通讯作者: Email: weizhidong1013@126.com (韦之栋); Email: shangguan@sjtu.edu.cn (上官文峰)

摘要: 固溶体策略可以在热力学上提高光催化性能，然而对固溶体催化剂载流子动力学的研究同样重要。本文基于能带结构调控成功合成了一系列Zn_xCd_1−xS固溶体，并通过飞秒瞬态吸收光谱(TAS)和密度泛函理论(DFT)研究了载流子动力学，揭示了Zn_xCd_1−xS固溶体中的混合直接-间接带隙跃迁机制。间接带隙表现出较低的载流子复合率，更重要的是它还可以作为载流子的捕获中心，从而提高电荷分离效率。因此，在可见光(> 420 nm)照射下，Zn_xCd_1−xS固溶体的析氢速率(1426.66 μmol h^–1)相较于纯CdS (129.83 μmol h^–1)提高了约11倍。本工作提出光催化性能的提升可能同时源于热力学和动力学两个方面，而载流子跃迁机制的改变是影响动力学的主要因素之一。

关键词:

English

Unveiling the mechanism of direct-to-indirect bandgap transition in the photocatalytic hydrogen evolution of Zn_xCd_1−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, weizhidong1013@126.com; Wenfeng Shangguan, shangguan@sjtu.edu.cn

Received Date: 16 June 2025
Accepted Date: 27 July 2025
Revised Date: 24 July 2025
Available Online: 15 January 2026

Abstract: 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_xCd_1−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_xCd_1−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_xCd_1−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.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

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

通讯作者: Email: weizhidong1013@126.com (韦之栋); Email: shangguan@sjtu.edu.cn (上官文峰)

English

Unveiling the mechanism of direct-to-indirect bandgap transition in the photocatalytic hydrogen evolution of Zn_xCd_1−xS solid solution

Corresponding author: Zhidong Wei, weizhidong1013@126.com; Wenfeng Shangguan, shangguan@sjtu.edu.cn

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揭示ZnxCd1−xS固溶体光催化析氢中的直接-间接带隙跃迁机制

通讯作者: Email: weizhidong1013@126.com (韦之栋); Email: shangguan@sjtu.edu.cn (上官文峰)

English

Unveiling the mechanism of direct-to-indirect bandgap transition in the photocatalytic hydrogen evolution of ZnxCd1−xS solid solution

Corresponding author: Zhidong Wei, weizhidong1013@126.com; Wenfeng Shangguan, shangguan@sjtu.edu.cn

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

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

Unveiling the mechanism of direct-to-indirect bandgap transition in the photocatalytic hydrogen evolution of Zn_xCd_1−xS solid solution

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs