Citation: Peipei Sun, Jinyuan Zhang, Yanhua Song, Zhao Mo, Zhigang Chen, Hui Xu. Built-in Electric Fields Enhancing Photocarrier Separation and H₂ Evolution[J]. Acta Physico-Chimica Sinica, ;2024, 40(11): 231100. doi: 10.3866/PKU.WHXB202311001 shu

Built-in Electric Fields Enhancing Photocarrier Separation and H₂ Evolution

Peipei Sun ¹ ,
Jinyuan Zhang ¹ ,
Yanhua Song ^2,, ,
Zhao Mo ^1,, ,
Zhigang Chen ¹ ,
Hui Xu ^1,,

1.
School of the Environment and Safety Engineering, Jingjiang College, Jiangsu University, Zhenjiang 212013, Jiangsu Province, China
2.
School of Environmental and Chemical Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003, Jiangsu Province, China

Corresponding author: Yanhua Song, songyh@just.edu.cn Zhao Mo, zhaomo@ujs.edu.cn Hui Xu, xh@ujs.edu.cn
Received Date: 1 November 2023
Revised Date: 13 December 2023
Accepted Date: 14 December 2023
Available Online: 25 December 2023
Fund Project: the National Natural Science Foundation of China 22378174the National Natural Science Foundation of China 21878134the National Natural Science Foundation of China 22208129the National Natural Science Foundation of China 22108110

The construct of the internal electric field (IEF) is recognized as an effective driver for promoting charge migration and separation to enhance photocatalytic performance. In this study, one-dimensional nanorods of Mn_0.2Cd_0.8S (MCS) co-doped with interstitial chlorine (Cl_int) and substitutional chlorine (Cl_sub) were designed and synthesized using a one-step solvothermal method. The incorporation of Cl_int and Cl_sub led to an unbalanced charge distribution and the formation of IEF in the MCS nanorods, contributing to the improvement of photogenerated carrier kinetic behavior. Through density functional theory (DFT) calculations, the effect of Cl_int and Cl_sub doping on the activity of the MCS was visually explained by examining differences in electronic structure, charge distribution and H₂ adsorption/desorption balance. Interestingly, the modulation of the energy band structure of MCS primarily resulted from the contribution of Cl_int, while Cl_sub playing a negligible role. Moreover, the Cl_sub further facilitated the optimization of Cl_int concerning the H₂ adsorption-desorption Gibbs free energy (ΔG_H*) of MCS. Ultimately, the ΔG_H* of 0.9 Cl-MCS favored H₂ production (1.14 vs. 0.17 eV), leading to a 9 times increase in photocatalytic H₂ production activity compared to MCS. This investigation presents a valuable approach for constructing IEF in bimetallic sulfide photocatalysts.
- Photocatalysis,
- H₂ production,
- Bimetallic sulfides,
- Internal electric fields,
- Gibbs free energy
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Built-in Electric Fields Enhancing Photocarrier Separation and H2 Evolution

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Built-in Electric Fields Enhancing Photocarrier Separation and H₂ Evolution