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

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): 2201008-0. doi: 10.3866/PKU.WHXB202201008 shu

具有光催化与光芬顿反应协同作用的2D/2D α-Fe₂O₃/g-C₃N₄ S型异质结用于高效降解四环素

王文亮 ^1, ,
张灏纯 ^1, ,
陈义钢 ^{2,
,} ,
史海峰 ^{1, 3,
,}

1.
江南大学理学院, 江苏无锡 214122
2.
南京医科大学附属无锡市第二人民医院普外科, 江苏无锡 214002
3.
南京大学固体微结构国家实验室, 南京 210093

通讯作者: 陈义钢, wuxichen2512@njmu.edu.cn
史海峰, hfshi@jiangnan.edu.cn

基金项目:
国家自然科学基金 22136002

国家自然科学基金 22172064

中央高校基本科研业务费 JUSRP51716A

南京大学固体微结构国家重点实验室开放课题 M34047

无锡转化医学中心项目 2020ZHYB10

无锡市卫健委重大科研项目 Z201901

摘要: 构建具有高效电荷迁移效率和丰富活性位点的异质结光催化体系是提升光芬顿反应速率的有效途径。本研究通过简单的水热法合成了2D/2D结构的α-Fe₂O₃/g-C₃N₄ S型异质结光芬顿催化剂，并使用X射线衍射仪技术(XRD)、透射电子显微镜(TEM)、傅立叶变换红外吸收光谱(FTIR)和紫外-可见吸收光谱(UV-Vis)等分析手段对α-Fe₂O₃/g-C₃N₄的晶体结构、微观结构、化学组分和光学性质进行了详细的表征。通过在可见光照射下降解四环素，评测了α-Fe₂O₃/g-C₃N₄的催化活性。结果表明，光催化反应与芬顿反应的协同作用使α-Fe₂O₃/g-C₃N₄ (1 : 1)展现出了优异的光芬顿催化活性：在可见光照射下，仅加入微量的双氧水便可辅助催化剂在20 min内对四环素的降解率达到78%，其降解速率分别是单一的α-Fe₂O₃和g-C₃N₄的3.5倍和5.8倍。α-Fe₂O₃/g-C₃N₄复合材料优异的催化活性得益于在2D/2D S型电荷迁移机制上构建的光芬顿催化体系。2D/2D S型异质结能够显著促进电子和空穴的传输与分离，并为催化剂提供较大的比表面积和丰富的活性位点，同时还能保持复合材料最佳的氧化还原能力。此外，光催化反应促进了Fe³⁺的还原，从而加速了芬顿反应中羟基自由基的产生。总之，本研究为构建高效、稳定的光芬顿催化体系提供了一条简单有效的途径。

关键词:

English

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

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: 05 January 2022
Accepted Date: 05 February 2022
Revised Date: 27 January 2022
Available Online: 15 July 2022
Fund Project:
the National Natural Science Foundation of China 22136002

the National Natural Science Foundation of China 22172064

Fundamental Research Funds for the Central Universities, China JUSRP51716A

National Laboratory of Solid State Microstructures, Nanjing University, China M34047

Wuxi Translational Medicine Center, China 2020ZHYB10

Major Scientific Research Projects of Wuxi Health Committee, China Z201901

Abstract: 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.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

具有光催化与光芬顿反应协同作用的2D/2D α-Fe₂O₃/g-C₃N₄ S型异质结用于高效降解四环素

通讯作者: 陈义钢, wuxichen2512@njmu.edu.cn
史海峰, hfshi@jiangnan.edu.cn

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

Corresponding author: Yigang Chen, wuxichen2512@njmu.edu.cn Haifeng Shi, hfshi@jiangnan.edu.cn

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具有光催化与光芬顿反应协同作用的2D/2D α-Fe2O3/g-C3N4 S型异质结用于高效降解四环素

通讯作者: 陈义钢, wuxichen2512@njmu.edu.cn 史海峰, hfshi@jiangnan.edu.cn

English