Citation: Haitao Wang, Lianglang Yu, Jizhou Jiang, Arramel, Jing Zou. S-Doping of the N-Sites of g-C₃N₄ to Enhance Photocatalytic H₂ Evolution Activity[J]. Acta Physico-Chimica Sinica, ;2024, 40(5): 230504. doi: 10.3866/PKU.WHXB202305047 shu

S-Doping of the N-Sites of g-C₃N₄ to Enhance Photocatalytic H₂ Evolution Activity

Haitao Wang ^{1, †} ,
Lianglang Yu ^{1, †} ,
Jizhou Jiang ^1,, ,
Arramel ² ,
Jing Zou ¹

1.
School of Chemistry and Environmental Engineering, School of Environmental Ecology and Biological Engineering, Key Laboratory of Green Chemical Engineering Process of Ministry of Education, Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education, Novel Catalytic Materials of Hubei Engineering Research Center, Wuhan Institute of Technology, Wuhan 430205, China
2.
Nano Center Indonesia, Jalan Raya PUSPIPTEK, South Tangerang, Banten 15314, Indonesia

Corresponding author: Jizhou Jiang, 027wit@163.com

^†

Received Date: 26 May 2023
Revised Date: 21 June 2023
Accepted Date: 21 June 2023
Available Online: 26 June 2023
Fund Project: the National Natural Science Foundation of China 62004143the Key R&D Program of Hubei Province, China 2022BAA084the Natural Science Foundation of Hubei Province, China 2021CFB133the National Key R&D Program of China 2022YFC3902703the Innovation Project of Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education, China LCX2021003the Open Research Fund of Key Laboratory of Material Chemistry for Energy Conversion and Storage (HUST), Ministry of Education, China 2021JYBKF05

The use of solar energy as an inexhaustible resource to conduct photocatalytic water splitting in hydrogen (H₂) production can alleviate the worldwide energy crisis and achieve carbon neutrality. However, research in photocatalytic H₂ evolution reaction (HER) is extremely challenging in terms of exploring the current development of an active and durable graphitic carbon nitride (g-C₃N₄)-based photocatalyst. Several parameters of pristine g-C₃N₄ require structural, physical, and chemical improvements, such as optimization of the surface area, electron transfer, and photo-generated carrier recombination, to render the g-C₃N₄ suitable for photocatalysis. In this study, the development of an efficient and robust S-doped g-C₃N₄ (S-g-CN) catalyst was pursued that involves doping nitrogen (N) active sites of g-C₃N₄ with sulfur (S) dopants via one-step calcination of the sulphate and melamine precursors. A combination of structural and spectroscopic fingerprints was established to distinctly determine the realization of S-doping onto the g-C₃N₄ structure. We obtained the optimum Gibbs free energy of adsorbed hydrogen (ΔG_H*) for S-g-CN at the S active sites, which is nearly zero (~0.26 eV), suggesting that the filled S dopants play an essential role in optimizing the adsorption and desorption processes of H-active intermediates. The results of atomic force and transmission electron microscopies (AFM and TEM) demonstrated that the produced S-g-CN catalyst has an ultrathin nanosheet structure with a lamellar thickness of approximately 2.5 nm. A subsequent N₂ sorption isotherms test revealed a substantial increase in the specific surface area after the integration of S dopants into the g-C₃N₄ nanoskeleton. Moreover, the incorporation of S atoms into the g-C₃N₄ significantly increased the carrier concentrations, improving the transfer, separation, as well as the oxidation and reduction abilities of the photo-generated electron-hole pairs. Leveraging the favorable material characteristics of the S-doped two-dimensional nanostructures, the resulting S-g-CN achieved a high H₂ evolution rate of 4923 μmol·g⁻¹·h⁻¹, which is 28 times higher than that of the pristine g-C₃N₄. Additionally, the developed S-g-CN possessed a high apparent quantum efficiency (3.64%) at visible-light irradiation. When compared to the recently reported S-doped g-C₃N₄-based photocatalysts, our optimal S-g-CN catalyst (S-CN_1.0) showed one of the best HER catalytic activities. Our rational design is based on an effective strategy that not only explored a promising HER photocatalyst but also aimed to pave the way for the development of other high-performance g-C₃N₄ based catalysts.
- Theoretical prediction,
- S-doping,
- g-C₃N₄,
- Hydrogen evolution,
- Photocatalysis
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沈阳化工大学材料科学与工程学院沈阳 110142

S-Doping of the N-Sites of g-C3N4 to Enhance Photocatalytic H2 Evolution Activity

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通讯作者: 陈斌, bchen63@163.com

S-Doping of the N-Sites of g-C₃N₄ to Enhance Photocatalytic H₂ Evolution Activity