穿透式碳纳米管电极的制备及其高效降解水中抗生素的性能和机理

王致远; 刘富强; 沈忱思; 李方; 刘亚男; 刘艳彪

doi:10.13198/j.issn.1001-6929.2021.09.26

穿透式碳纳米管电极的制备及其高效降解水中抗生素的性能和机理

doi: 10.13198/j.issn.1001-6929.2021.09.26

王致远^1,,
刘富强¹,
沈忱思^{1, 2},
李方^{1, 2},
刘亚男^{1, 2},
刘艳彪^{1, 2, ,}

1.
东华大学环境科学与工程学院, 国家环境保护纺织工业污染防治工程技术中心, 上海 201620
2.
上海污染控制与生态安全研究院, 上海 200092

基金项目:

国家自然科学基金项目 52170068

详细信息

作者简介:
王致远(1998-), 男, 江苏泰州人, 2202052@mail.dhu.edu.cn

通讯作者:
刘艳彪(1982-), 男, 上海人, 教授, 博士, 博导, 主要从事电活性分离膜净水技术研究, yanbiaoliu@dhu.edu.cn

中图分类号: X703.1
计量
- 文章访问数: 233
- HTML全文浏览量: 77
- PDF下载量: 47
- 被引次数: 0
出版历程
- 收稿日期: 2021-07-16
- 修回日期: 2021-09-24

Efficient Degradation of Antibiotics by Flow-Through Electro-Fenton System Based on Modified Carbon Nanotubes Electrode: Performance and Mechanism

WANG Zhiyuan^1
,,
LIU Fuqiang¹,
SHEN Chensi^{1, 2},
LI Fang^{1, 2},
LIU Yanan^{1, 2},
LIU Yanbiao^{1, 2
, ,}

1.
Textile Pollution Controlling Engineering Center of Ministry of Environmental Protection, College of Environmental Science and Engineering, Donghua University, Shanghai 201620, China
2.
Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China

Funds:

National Natural Science Foundation of China 52170068

摘要

摘要: 为实现水中四环素类抗生素的高效降解，本文设计开发了一种基于电活性碳纳米管(CNT)电极的穿透式电芬顿系统，采用水热法制得纳米铁和二硫化钼共修饰的CNT阴极材料(Fe-MoS₂@CNT)，分析不同因素对电芬顿催化降解四环素性能的影响. 结果表明：基于改性CNT电极的穿透式电芬顿系统对四环素表现出良好的去除性能，电压和流速等对四环素的降解动力学具有显著影响. 该系统的最优试验条件：Fe掺杂量为0.3 mmol/L、外加电压为-2.5 V、流速为0.85 cm³/(min·cm²). 在最优试验条件下，反应60 min内四环素的降解率可达到95%，羟基自由基为主导的活性物种. 连续运行240 min后，该系统对四环素的降解率仍保持在85%以上，且在实际湖水环境水基质中对四环素降解率也可达到87.2%. 研究显示，Fe-MoS₂@CNT膜电极具有优异的催化性能及可重复利用性，可以高效降解水中四环素类抗生素.
- 穿透式电芬顿 /
- 碳纳米管 /
- 羟基自由基 /
- 四环素
Abstract: A flow-through electro-Fenton system based on an electroactive carbon nanotube (CNT) filter was designed and demonstrated for efficient degradation of antibiotic tetracycline. The key to this technology was a CNT cathode functionalized with iron and molybdenum disulfide (Fe-MoS₂@CNT). The effects of different operational parameters on the degradation of tetracycline were systematically examined. The results showed that the flow-through electro-Fenton system had an excellent performance for tetracycline degradation. The applied voltage and flow rate significantly affected the degradation kinetics of tetracycline. The optimal experimental conditions of the system were Fe loading of 0.3 mmol/L, applied voltage of -2.5 V, and flow rate of 0.85 cm³/(min·cm²). Under these conditions, the degradation efficiency of tetracycline reached 95% after 60 min reaction, and HO^· was identified as the dominant reactive species. After four continuous running cycles, the degradation efficiency of tetracycline was still >85%. A removal efficiency of 87.2% could be achieved in the tetracycline-spiked lake water sample. The findings in this study demonstrate that the Fe-MoS₂@CNT filter has excellent catalytic performance and desirable reusability, and can be used to remove other refractory organic contaminants in water.
- flow-through electro-Fenton /
- carbon nanotubes /
- hydroxyl radical /
- tetracycline

HTML全文

图 1 电过滤装置原理示意图以及反应器上部、内部和Fe-MoS₂@CNT膜电极的实物图

Figure 1. Schematics of electroactive filtration apparatus and digital pictures of the filtration device and the Fe-MoS₂@CNT cathode

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图 2 Fe-MoS₂@CNT膜电极的表征

Figure 2. Characterization of the Fe-MoS₂@CNT filter

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图 3 Fe-MoS₂@CNT膜电极的XPS谱图

Figure 3. XPS survey pattern of the Fe-MoS₂@CNT filter

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图 4 不同电压对H₂O₂通量的影响

Figure 4. Effects of different voltages on H₂O₂ flux

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图 5 不同影响因素对四环素降解效果的影响

Figure 5. Effects of different factors on tetracycline degradation

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图 6 Fe-MoS₂@CNT膜电极的重复利用性和在环境水基质中对四环素的降解率

Figure 6. Reusability of the Fe-MoS₂@CNT filter and degradation efficiency of tetracycline in environmental water

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图 7 四环素在Fe-MoS₂@CNT膜电极中降解的可能机制

Figure 7. Possible degradation mechanism of tetracycline in the Fe-MoS₂@CNT filter

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图 8 四环素在穿透式电芬顿系统中的降解路径

Figure 8. Proposed tetracycline degradation pathway in the electro-Fenton system

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表 1 不同环境水基质的特性

Table 1. Specific information for the different water samples

环境水基质	pH	溶解氧浓度/(mmol/L)	TOC浓度/(mg/L)	电导率/(μS/cm)
自来水	7.83	0.21	1.62	518.67
湖水	8.07	0.18	95.23	682.75

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