Electrocatalytic Degradation of Wastewater by Polymer-based Carbon Nanomembranes and Mechanism

doi:10.6023/A23010001

Acta Chimica Sinica ›› 2023, Vol. 81 ›› Issue (4): 420-430.DOI: 10.6023/A23010001 Previous Articles

Review

高分子聚合物基碳纳米膜的电催化降解污水性能及机理

张慧颖^a^,^b^,^c, 于淑艳^a^,^b^,^c^,^*(), 李从举^a^,^b^,^c^,^*()

a 北京科技大学能源与环境工程学院北京 100083
b 北京科技大学北京市工业典型污染物资源化处理重点实验室北京 100083
c 北京市高校节能与环保工程研究中心北京 100083

投稿日期:2023-01-01 发布日期:2023-03-23

作者简介:

张慧颖, 于2022年获得青岛科技大学学士学位, 2022年至今在于淑艳老师的指导下攻读硕士学位. 研究兴趣是探究静电纺丝电催化高效碳纤维微滤膜研制及其降解废水性能.

于淑艳讲师, 硕士生导师. 于2013获得山东大学双学士学位, 2018年获得新加坡南洋理工大学博士学位, 2020年获得清华大学博士后, 现为北京科技大学讲师. 研究兴趣是探究静电纺丝电催化高效碳纤维微滤膜研制及其降解废水性能.

李从举教授, 博士生导师. 于2004年获得中国科学院化学研究所博士学位, 现任北京科技大学教授. 2017年获得国家“万人计划”科技创新领军人才称号. 研究重点是环境纳米材料与技术.

基金资助:
国家自然科学基金(52103070); 中央高校基本科研基金(FRF-TP-20-057A1); 中央高校基本科研基金(06500100); “万人计划”——国家高层次人才专项支持计划

Electrocatalytic Degradation of Wastewater by Polymer-based Carbon Nanomembranes and Mechanism

Huiying Zhang^a^,^b^,^c, Shuyan Yu^a^,^b^,^c^,^*(), Congju Li^a^,^b^,^c^,^*()

a School of Energy and Environmental Engineering, University of Science and Technology Beijing, Beijing 100083, China
b Beijing Key Laboratory of Resource-oriented Treatment of Industrial Pollutants, Beijing 100083, China
c Energy Conservation and Environmental Protection Engineering Research Center in Universities of Beijing, Beijing 100083, China

Received:2023-01-01 Published:2023-03-23
Contact: * E-mail: yushuyan@ustb.edu.cn; congjuli@126.com
Supported by:
National Natural Science Foundation of China(52103070); Fundamental Research Funds for the Central Universities(FRF-TP-20-057A1); Fundamental Research Funds for the Central Universities(06500100); “Ten thousand plan”-National High-level personnel of special support program

Advanced electrocatalytic oxidation technology generally uses plate electrodes, because the hindered mass transfer has disadvantages of incomplete degradation, which limits the application of electrocatalytic degradation of pollutants. As a new type of electrode, porous carbon nanomembranes can effectively improve the mass transfer efficiency, thereby overcoming the shortcomings of traditional technology, it have been widely used in recent years. In this paper, the methods for preparing carbon films are reviewed, including electrospinning technology (EST), chemical vapor deposition (CVD) and template method, the principles and operating methods of the different techniques are introduced separately, and examples of the practical application of each method are given. Among them, electrospinning technology has the advantages of facilitating the modification of carbon films and the preparation of oriented carbon membranes. Secondly, the research on the electrocatalytic degradation of wastewater containing antibiotics, dye molecules and other organic compounds by carbon membrane is summarized, the universality of electrocatalysis is illustrated from the effective degradation results of carbon membranes for different organic compounds, the high efficiency, cleanliness and reproducibility of carbon membranes as electrodes for electrocatalytic degradation of wastewater are further demonstrated by different studies. These studies have further improved the performance of carbon membrane as electrodes by adding metals, metal oxides and metal-organic frameworks to the carbon membranes. Finally, the mechanism of electrochemical advanced oxidation, effect of electrode and main detection methods of free radicals are described, the mechanism of electrochemical advanced oxidation is introduced in terms of direct and indirect oxidation, and specific demonstration is made through equations, the possible electrode effects and their influence on electrocatalytic degradation of wastewater are cited as example. The methods of detecting free radicals are mainly introduced as quenching method and probe method, the principles and controversies are explained, and the development of carbon film electrocatalytic degradation of wastewater is prospected.

Key words: polymer-based, carbon membrane, electrochemical oxidation, wastewater treatment, mechanism

Cite this article

Huiying Zhang, Shuyan Yu, Congju Li. Electrocatalytic Degradation of Wastewater by Polymer-based Carbon Nanomembranes and Mechanism[J]. Acta Chimica Sinica, 2023, 81(4): 420-430.

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Fig. & Tab. 22

Figure 1. Develpmpent history of carbon nanomembranes

Figure 2. SEM (a) and TEM (b) images of Ni-doped carbon nanofibers[21]

Figure 3. FT-IR (a) and XRD (b) images of CNF and MOFs/CNF[22]

Figure 4. Schematic diagram of electrospinning device[29]

Figure 5. (a) Electrospinning device (b) SEM diagram oriented to SrTiO3/PAN[33]

Figure 6. Schematic diagram of carbon nanofiber nucleation and growth prepared by CVD[35-36]

Figure 7. Schematic diagram of the template method[41]

Figure 8. Cross-sectional schematic of synthesized PAN nanofibers[42]

制备方法	优势	挑战
EST	可以制备取向性的碳纳米纤维; 生产出的纳米纤维直径小, 利于反应进行; 设备成本低; 制备出的纳米纤维表面光滑且粗细均匀	对其进行改性时需要考虑到纳米纤维的直径限制; 反应时溶剂需要进一步处理; 纺丝过程受到纺丝液、电压、接收距离等的影响
CVD	生长条件可控; 制备出的碳纳米纤维强度高; 沉积速率高; 制备出的材料纯度高	反应后的余气中可能含有有毒物质; 设备成本高
模板法	制备方法简单	碳纳米纤维直径大; 密度低

Table 1. Comparison of advantages and challenges of different methods

Figure 9. Application of carbon film electrocatalytic degradation of wastewater

Figure 10. Schematic diagram of Fe/Co-CNFs prepared by electrospinning (a) and the carbonization process (b)[11]

Figure 11. Degradation effect of recovered Fe/Co-CNFs on tetracyclines and SEM diagram of Fe/Co-CNFs recovered ten times[11]

Figure 12. Schematic diagram of the degradation of NOR by rGO@Ti/SnO2-Sb[12]

Figure 13. MO degradation curves of ACF, e-ACF and e-CNT/ACF as electrode[48]

Figure 14. SEM images of NPs (a), NCs (b) and NFs (c, d)[49]

Figure 15. Degradation mode (a) and path (b) of TCS[56]

Figure 16. Cyclic voltammetry of nanofibers containing 0% MnAc at different urea concentrations (a) and nanofibers containing different Mn content in 1 mol/L urea solution (b) at 1000 ℃[58]

电极	有机物	初始浓度	降解效果	文献
Fe/Co-CNFs	TC	30 mg/L	12 h去除率100.0%	[11]
ACFs	TC/OTC	40 mg/L	2 h去除率80%	[45]
rGO@Ti/SnO₂-Sb	NOR	100 mg/L	1.5 h去除率96.3%	[12]
G/SnO₂/CFs	SMX	15 mg/L	8 h去除率85%	[46]
e-CNT/ACF	MO	25 mg/L	1 h去除率90%	[48]
BTO NFs	RhB	7.5 mg/L	75 min去除率99%	[49]
TiO₂/CM	MB	200 mg/L	12 h去除率99.9%	[1]
CNTs-C/PTFE	TCS	50 mg/L	1 h去除率98%	[56]
Cu-rGO-PC	DCF	20 mg/L	1 h去除率100%	[57]

Table 2. Performance comparison of different electrodes

Figure 17. Schematic diagram of electrochemical oxidation mechanism (Direct oxidation: blue, indirect oxidation: yellow)[61-62]

Figure 18. Thermal imaging image of electrode surface before (a) and after 120 min (b) of electrolysis and thermal imaging image of the bulk solution before (c) and after 120 min (d) of electrolysis[65]

Figure 19. Free radical scavenging test in electric fenton system [71]

Figure 20. Consumption of PMS, ATZ, PMD in synthetic solution (a) and PMS, ?OH, SO4?? exposure (b)[72]

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高分子聚合物基碳纳米膜的电催化降解污水性能及机理

Electrocatalytic Degradation of Wastewater by Polymer-based Carbon Nanomembranes and Mechanism

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