Research progress in photoelectrocatalytic degradation of antibiotics in wastewater

doi:10.19965/j.cnki.iwt.2022-0802

Abstract

Abstract:

The abuse of antibiotics causes serious environmental pollution and endangers human health. Photoelectrocatalytic technology（PEC） uses photocatalytic reactions assisted electrochemical to suppress the recombination of photo generated electron-hole by applying an external bias to the photocatalyst under light，which can increase the concentration of free radicals and significantly improve the organic matter degradation rate. PEC has the advantages of environmental protection，energy conservation，strong oxidation ability and easy operation，and has become one of the most promising advanced oxidation technologies for removing refractory pollutants such as antibiotics. The progress of PEC degrading antibiotics was comprehensively reviewed，and the principle of PEC was introduced. The modification methods and properties of electrode materials were summarized. The latest applications of PEC degrading antibiotics and the effects of bias potential，pH，electrolyte，light source on the antibiotic degradation rate in the experiment were expounded. Finally，the prospects and challenges of PEC degrading antibiotics were summarized，in order to provide a reference for the application of photoelectrocatalytic technology to efficiently treat antibiotic wastewater.

Key words: photoelectrocatalysis, electrode material, antibiotics, advanced oxidation

摘要：

抗生素滥用造成了严重的环境污染并危害人体健康。光电催化技术（PEC）以电化学辅助光催化反应，在光照下通过向光催化剂施加外部偏压抑制光生电子-空穴对的复合，提高自由基浓度，以此显著提高系统对有机物的降解速率，具有环保节能、氧化能力强、操作方便等优势，已成为去除抗生素等难降解污染物最有前景的高级氧化技术之一。对PEC降解抗生素的进展进行了全面综述，介绍了PEC原理，重点总结了电极材料改性方法及其性能，阐述了PEC降解抗生素的最新应用及降解中偏置电压、pH、电解液、光源等对抗生素降解率的影响，最后对PEC降解抗生素的前景和挑战进行了总结和展望，以期为应用光电催化技术高效处理抗生素废水的研究提供参考。

关键词: 光电催化, 电极材料, 抗生素, 高级氧化

CLC Number:

X703

Huixia ZHANG, Lingzhi ZHU, Lishan ZHOU, Chenxin XIE, Chenglei ZHANG, Enshan HAN. Research progress in photoelectrocatalytic degradation of antibiotics in wastewater[J]. Industrial Water Treatment, 2023, 43(11): 104-113.

张会霞, 朱令之, 周立山, 谢陈鑫, 张程蕾, 韩恩山. 光电催化降解废水中抗生素的研究进展[J]. 工业水处理, 2023, 43(11): 104-113.

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URL: https://www.iwt.cn/EN/10.19965/j.cnki.iwt.2022-0802

https://www.iwt.cn/EN/Y2023/V43/I11/104

Figures/Tables 3

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光阳极	对电极	改性方式	抗生素废水	操作参数	降解效果		参考文献
光阳极	对电极	改性方式	抗生素废水	操作参数	反应时间/min	降解率/%	参考文献
I-P/TiO₂	不锈钢	共掺杂	100 mL、10 mg/L四环素废水	400 W金属卤素灯，E=1.4 V（vs. NHE），pH=11.04，电解质0.1 mol/L Na₂SO₄	180	99.7	〔31〕
Ar-Fe₂O₃/Ti₃ ⁺-TiO₂纳米管	Pt片	自掺杂、金属有机框架构建异质结构	250 mL、20 mg/L 四环素废水	300 W氙灯，E=2 V（vs. Ag/AgCl），pH=6，电解质0.05 mol/L Na₂SO₄	90	100	〔32〕
BiVO₄/ZnO纳米棒	Pt片	构建三维珊瑚结构、异质结构	50 mL、20 mg/L四环素废水	300 W氙灯，E=1.2 V（vs. Ag/AgCl），电解质0.1 mol/L Na₂SO₄	60	95.4	〔33〕
Bi₂O₃/WO₃	不锈钢	构建花状p-n异质结	50 mL、10 mg/L诺氟沙星废水	300 W氙灯，E=1.0 V（vs. SCE），电解质0.1 mol/L Na₂SO₄	180	88.4	〔34〕
Ti/SnO₂-Sb	炭黑/不锈钢	构建双光电催化耦合系统	140 mL抗生素制药厂废水	紫外灯，J=7.06 mA/cm²，pH=7	120	95.6	〔36〕
MoS₂/CuInS₂	不锈钢	构建Z型异质结	60 mL、30 mg/L四环素废水	300 W石英卤素灯，E=0.2 V（vs. Ag/AgCl），电解质0.1 mol/L Na₂SO₄	180	89	〔37〕
ZnSe-CdSe/MoS₂	Pt片	构建四元半导体核壳结构	50 mL、10 mg/L阿莫西林废水	300 W氙灯，E=0.5 V（vs. Ag/AgCl），电解质0.1 mol/L Na₂SO₄	30	100	〔40〕
Ag₃PO₄/BiVO₄	Pt片	构建异质结	5 mg/L诺氟沙星废水	300 W氙灯，E=0.5 V（vs. SCE），电解质 0.01 mol/L NaClO₄	90	100	〔41〕
BiOBr纳米片阵列	Pt片	形貌改性	10 mL、15 mg/L环丙沙星废水	500 W氙灯，E=0.9 V（vs. Ag/AgCl），pH=8.96，电解质0.1 mol/L Na₂SO₄	180	96.8	〔42〕
MoS₂/rGO/Bi₂S₃@碳纤	BiOBr@碳纤	构建Z型异质结	100 mL、20 mg/L四环素废水	350 W氙灯，外部电阻500 Ω，pH=2，电解质0.5 mol/L Na₂SO₄	60	97.7	〔44〕
rGO/g-C₃N₄/TiO₂	同光阳极	采用双室光电催化	80 mL、40 mg/L土霉素废水	150 W氙灯，E=1.2 V（vs. SCE），电解质0.1 mol/L Na₂SO₄	60	69.37	〔47〕
g-C₃N₄/MIL- 101（Fe）	石墨片	构建异质结	100 mL、10 mg/L环丙沙星废水	12 W LED灯，I=50 mA，pH=3.11，电解质0.05 mol/L Na₂SO₄	240	87.55	〔48〕
rGO/AgCl	Pt片	构建量子点	100 mL、20 mg/L四环素废水	300 W氙灯，E=1.5 V（vs. Ag/AgCl），电解质0.1 mol/L Na₂SO₄	120	85.2	〔49〕
YFeO₃	活性炭纳米纤维	光电催化和光电子-Fenton协同效应	500 mL、10 mg/L磺胺甲嘧啶废水	紫外灯，E=25 V，pH=3，电解质7 mmol/L Na₂SO₄	60	83	〔54〕
BiVO₄	聚多巴胺改性碳毡	激活过氧单硫酸盐	160 mL、8 mg/L氧氟沙星废水	300 W氙灯，E=1.5 V（vs. Ag/AgCl），pH=5，电解质2 mmol/L过氧单硫酸盐	120	100	〔55〕

光阳极	对电极	改性方式	抗生素废水	操作参数	降解效果		参考文献
光阳极	对电极	改性方式	抗生素废水	操作参数	反应时间/min	降解率/%	参考文献
I-P/TiO₂	不锈钢	共掺杂	100 mL、10 mg/L四环素废水	400 W金属卤素灯，E=1.4 V（vs. NHE），pH=11.04，电解质0.1 mol/L Na₂SO₄	180	99.7	〔31〕
Ar-Fe₂O₃/Ti₃ ⁺-TiO₂纳米管	Pt片	自掺杂、金属有机框架构建异质结构	250 mL、20 mg/L 四环素废水	300 W氙灯，E=2 V（vs. Ag/AgCl），pH=6，电解质0.05 mol/L Na₂SO₄	90	100	〔32〕
BiVO₄/ZnO纳米棒	Pt片	构建三维珊瑚结构、异质结构	50 mL、20 mg/L四环素废水	300 W氙灯，E=1.2 V（vs. Ag/AgCl），电解质0.1 mol/L Na₂SO₄	60	95.4	〔33〕
Bi₂O₃/WO₃	不锈钢	构建花状p-n异质结	50 mL、10 mg/L诺氟沙星废水	300 W氙灯，E=1.0 V（vs. SCE），电解质0.1 mol/L Na₂SO₄	180	88.4	〔34〕
Ti/SnO₂-Sb	炭黑/不锈钢	构建双光电催化耦合系统	140 mL抗生素制药厂废水	紫外灯，J=7.06 mA/cm²，pH=7	120	95.6	〔36〕
MoS₂/CuInS₂	不锈钢	构建Z型异质结	60 mL、30 mg/L四环素废水	300 W石英卤素灯，E=0.2 V（vs. Ag/AgCl），电解质0.1 mol/L Na₂SO₄	180	89	〔37〕
ZnSe-CdSe/MoS₂	Pt片	构建四元半导体核壳结构	50 mL、10 mg/L阿莫西林废水	300 W氙灯，E=0.5 V（vs. Ag/AgCl），电解质0.1 mol/L Na₂SO₄	30	100	〔40〕
Ag₃PO₄/BiVO₄	Pt片	构建异质结	5 mg/L诺氟沙星废水	300 W氙灯，E=0.5 V（vs. SCE），电解质 0.01 mol/L NaClO₄	90	100	〔41〕
BiOBr纳米片阵列	Pt片	形貌改性	10 mL、15 mg/L环丙沙星废水	500 W氙灯，E=0.9 V（vs. Ag/AgCl），pH=8.96，电解质0.1 mol/L Na₂SO₄	180	96.8	〔42〕
MoS₂/rGO/Bi₂S₃@碳纤	BiOBr@碳纤	构建Z型异质结	100 mL、20 mg/L四环素废水	350 W氙灯，外部电阻500 Ω，pH=2，电解质0.5 mol/L Na₂SO₄	60	97.7	〔44〕
rGO/g-C₃N₄/TiO₂	同光阳极	采用双室光电催化	80 mL、40 mg/L土霉素废水	150 W氙灯，E=1.2 V（vs. SCE），电解质0.1 mol/L Na₂SO₄	60	69.37	〔47〕
g-C₃N₄/MIL- 101（Fe）	石墨片	构建异质结	100 mL、10 mg/L环丙沙星废水	12 W LED灯，I=50 mA，pH=3.11，电解质0.05 mol/L Na₂SO₄	240	87.55	〔48〕
rGO/AgCl	Pt片	构建量子点	100 mL、20 mg/L四环素废水	300 W氙灯，E=1.5 V（vs. Ag/AgCl），电解质0.1 mol/L Na₂SO₄	120	85.2	〔49〕
YFeO₃	活性炭纳米纤维	光电催化和光电子-Fenton协同效应	500 mL、10 mg/L磺胺甲嘧啶废水	紫外灯，E=25 V，pH=3，电解质7 mmol/L Na₂SO₄	60	83	〔54〕
BiVO₄	聚多巴胺改性碳毡	激活过氧单硫酸盐	160 mL、8 mg/L氧氟沙星废水	300 W氙灯，E=1.5 V（vs. Ag/AgCl），pH=5，电解质2 mmol/L过氧单硫酸盐	120	100	〔55〕

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