高分子聚合物基碳纳米膜的电催化降解污水性能及机理

doi:10.6023/A23010001

化学学报 ›› 2023, Vol. 81 ›› Issue (4): 420-430.DOI: 10.6023/A23010001 上一篇

综述

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

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摘要/Abstract

目前的电催化高级氧化技术普遍使用平板电极, 因为传质受阻在降解污染物方面具有降解不彻底的缺点, 限制了其在电催化降解污染物的应用. 多孔碳纳米膜作为一种新型电极, 因其较大的比表面积, 提供较多反应活性位点, 可以有效地改善传质效率, 从而克服此传统技术的缺点, 在近年来得到广泛应用. 本文首先综述了使用高分子聚合物制备碳纳米膜的方法, 主要包括静电纺丝技术(EST)、化学气相沉积法(CVD)和模板法, 分别介绍了每种技术的原理和操作方法, 并展示每种方法的实际应用的实例. 其中静电纺丝技术具有可以制备取向碳纳米纤维并有助于碳纳米纤维改性的优点. 其次总结了碳膜电催化降解含抗生素、染料分子和其他有机物的污水的研究进展, 对不同条件下电催化降解有机物的效果进行综述, 大部分研究均通过在碳纳米膜上添加金属、金属氧化物和金属有机框架(MOF)来使电极的性能得到优化. 最后阐述了电化学高级氧化的机理、电极效应及主要的检测自由基的方法, 分别从直接氧化和间接氧化两个方面介绍了电化学高级氧化的机理, 并通过公式进行具体论证; 列举了电催化过程中可能产生的电极效应对有机物降解的影响; 检测自由基的方法主要总结了淬灭法和探针法, 并阐述了其原理和争议, 并对碳纳米膜电催化降解废水的发展进行展望.

关键词: 高分子聚合物基, 碳膜, 电化学氧化, 污水处理, 机理

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

引用此文

张慧颖, 于淑艳, 李从举. 高分子聚合物基碳纳米膜的电催化降解污水性能及机理[J]. 化学学报, 2023, 81(4): 420-430.

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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图/表 22

图1. 碳纳米膜的发展历史

Figure 1. Develpmpent history of carbon nanomembranes

图2. Ni掺杂的碳纳米纤维的SEM (a)和TEM (b)图像[21]

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

图3. CNF和MOFs/CNF的FT-IR (a)和XRD (b)图[22]

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

图4. 静电纺丝装置示意图[29]

Figure 4. Schematic diagram of electrospinning device[29]

图5. 静电纺丝装置(a)和取向SrTiO3/PAN的SEM图(b)[33]

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

图6. CVD制备碳纳米纤维成核和生长示意图[35-36]

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

图7. 模板法示意图[41]

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

图8. 合成的PAN纳米纤维的横截面示意图[42]

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

表1. 不同方法的优势和挑战对比

Table 1. Comparison of advantages and challenges of different methods

图9. 碳膜电催化降解污水的应用

Figure 9. Application of carbon film electrocatalytic degradation of wastewater

图10. 静电纺丝制备Fe/Co-CNFs (a)和Fe/Co-CNFs的碳化过程(b)示意图[11]

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

图11. 回收的Fe/Co-CNFs对于四环素的降解效果及回收10次的Fe/Co-CNFs SEM图[11]

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

图12. rGO@Ti/SnO2-Sb降解NOR原理图[12]

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

图13. ACF、e-ACF和e-CNT/ACF作为电极时的MO降解曲线[48]

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

图14. NPs (a), NCs (b)和NFs (c, d)的SEM图[49]

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

图15. TCS的降解方式(a)及路径(b)[56]

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

图16. 1000 ℃下煅烧含有0% MnAc的纳米纤维在不同尿素浓度下(a)和含有不同Mn含量的纳米纤维在1 mol/L尿素溶液中(b)的循环伏安图[58]

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]

表2. 不同电极的性能对比

Table 2. Performance comparison of different electrodes

图17. 电化学氧化机理示意图(直接氧化: 蓝色, 间接氧化: 黄色)[61-62]

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

图18. 电极表面电解120 min前(a)、后(b)和主体溶液电解120 min前(c)、后(d)的热成像图[65]

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]

图19. 电fenton系统中的自由基清除测试[71]

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

图20. PMS、ATZ、PMD在合成溶液中的消耗(a)及PMS、?OH和SO4??的暴露量(b)[72]

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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