Citation: Wenliang Wang, Haochun Zhang, Yigang Chen, Haifeng Shi. Efficient Degradation of Tetracycline via Coupling of Photocatalysis and Photo-Fenton Processes over a 2D/2D α-Fe₂O₃/g-C₃N₄ S-Scheme Heterojunction Catalyst[J]. Acta Physico-Chimica Sinica, ;2022, 38(7): 220100. doi: 10.3866/PKU.WHXB202201008 shu

Efficient Degradation of Tetracycline via Coupling of Photocatalysis and Photo-Fenton Processes over a 2D/2D α-Fe₂O₃/g-C₃N₄ S-Scheme Heterojunction Catalyst

Wenliang Wang ¹ ,
Haochun Zhang ¹ ,
Yigang Chen ^2,, ,
Haifeng Shi ^{1, 3,,}

1.
School of Science, Jiangnan University, Wuxi 214122, Jiangsu Province, China
2.
Department of General Surgery, The Affiliated Wuxi No. 2 People's Hospital of Nanjing Medical University, Wuxi 214002, Jiangsu Province, China
3.
National Laboratory of Solid State Microstructures, Nanjing University, Nanjing 210093, China

Corresponding author: Yigang Chen, wuxichen2512@njmu.edu.cn Haifeng Shi, hfshi@jiangnan.edu.cn
Received Date: 5 January 2022
Revised Date: 27 January 2022
Accepted Date: 5 February 2022
Available Online: 10 January 2022
Fund Project: the National Natural Science Foundation of China 22136002the National Natural Science Foundation of China 22172064Fundamental Research Funds for the Central Universities, China JUSRP51716ANational Laboratory of Solid State Microstructures, Nanjing University, China M34047Wuxi Translational Medicine Center, China 2020ZHYB10Major Scientific Research Projects of Wuxi Health Committee, China Z201901

Graphitic carbon nitride (g-C₃N₄) has been widely used as a potential photocatalytic material for the removal of tetracycline from water. However, the poor visible light absorption ability and high recombination rate of the photogenerated charge significantly inhibit the catalytic activity of g-C₃N₄. Therefore, facile methods to improve the photocatalytic efficiency of g-C₃N₄ need to be developed. Hematite (α-Fe₂O₃), which has a good visible light absorption and corrosion resistance, is often used for photocatalysis and photo-Fenton reactions. Therefore, a two-dimension/two-dimension (2D/2D) S-scheme heterojunction constructed of g-C₃N₄ and α-Fe₂O₃ nanosheets could be expected to improve the degradation efficiency of tetracycline. In this study, 2D/2D S-scheme α-Fe₂O₃/g-C₃N₄ photo-Fenton catalysts were prepared using a hydrothermal strategy. The photo-Fenton catalytic activity of α-Fe₂O₃/g-C₃N₄ (α-Fe₂O₃ 50% (w)) was significantly improved by the addition of a small amount of H₂O₂, removing 78% of tetracycline within 20 min, which was approximately 3.5 and 5.8 times the removal achieved using α-Fe₂O₃ and g-C₃N₄, respectively. The high catalytic activity was attributed to the synergy between the photocatalysis and Fenton reaction promoted by the continuous Fe³⁺/Fe²⁺ conversion over the 2D/2D S-scheme heterojunction. The 2D/2D S-scheme heterojunction was crucial in the fabrication of the α-Fe₂O₃/g-C₃N₄ photocatalyst with a large surface area, adequate active sites, and strong oxidation-reduction capability. Furthermore, the photo-Fenton reaction provided additional hydroxyl radicals for the degradation of tetracycline with the aid of H₂O₂. The excess reaction product (Fe³⁺) was reduced to Fe²⁺ by the photogenerated electrons from the conduction band of α-Fe₂O₃. The resulting Fe²⁺ could participate in the photo-Fenton reaction. The morphological structures of α-Fe₂O₃/g-C₃N₄ were analyzed using transmission electron microscopy to demonstrate the formation of a 2D/2D structure with face-to-face contact, and the optical properties of the composites were measured using ultraviolet-visible diffuse reflectance spectroscopy. α-Fe₂O₃/g-C₃N₄ possessed a significantly improved visible light absorption compared to g-C₃N₄. Five sequential cyclic degradation tests and X-ray diffraction (XRD) patterns obtained before and after the reaction showed that the α-Fe₂O₃/g-C₃N₄ composites possessed stable photo-Fenton catalytic activity and crystal structures. Transient photocurrent responses of α-Fe₂O₃/g-C₃N₄ demonstrated that the prepared composites exhibited a higher charge transfer efficiency compared to that of single α-Fe₂O₃ and g-C₃N₄. In addition, according to the photoluminescence analysis and active species trapping experiments, a possible S-scheme heterojunction charge transfer process in the photo-Fenton catalytic reaction was proposed. This study provided a promising method for the construction of a high-performance photo-Fenton catalytic system to remove antibiotics from wastewater.
- Photocatalysis,
- Fenton reaction,
- Catalytic activity,
- S-scheme heterojunction,
- 2D/2D interface
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Efficient Degradation of Tetracycline via Coupling of Photocatalysis and Photo-Fenton Processes over a 2D/2D α-Fe2O3/g-C3N4 S-Scheme Heterojunction Catalyst

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通讯作者: 陈斌, bchen63@163.com

Efficient Degradation of Tetracycline via Coupling of Photocatalysis and Photo-Fenton Processes over a 2D/2D α-Fe₂O₃/g-C₃N₄ S-Scheme Heterojunction Catalyst