碳纳米管掺杂PbO<sub>2</sub>复合电极的制备及其催化氧化双酚A

吴梦怡; 龙昕; 高丛浩; 秦晓; 陈月; 唐玉霖

doi:10.13205/j.hjgc.202104009

碳纳米管掺杂PbO₂复合电极的制备及其催化氧化双酚A

doi: 10.13205/j.hjgc.202104009

吴梦怡¹,
龙昕¹,
高丛浩¹,
秦晓²,
陈月³,
唐玉霖^1, ,

1. 同济大学环境科学与工程学院污染控制与资源化利用国家重点试验室, 上海 200092;
2. 同济大学城市污染控制国家工程研究中心, 上海 200092;
3. 河北建设集团安装工程有限公司, 河北保定 071000

基金项目:

国家自然基金"基于废塑料的磁性纳米碳材料构筑及其催化机理研究"（21776224）。

详细信息

作者简介:
吴梦怡(1996-),女,硕士研究生,主要研究方向为水处理理论与技术。my.wu@tongji.edu.cn

通讯作者:
唐玉霖(1977-),男,博士,教授,主要研究方向为水处理理论与技术。tangtongji@126.com

计量
- 文章访问数: 404
- HTML全文浏览量: 42
- PDF下载量: 31
- 被引次数: 0
出版历程
- 收稿日期: 2020-03-16
- 网络出版日期: 2021-07-21

FABRICATION OF CARBON NANOTUBE-DOPED PbO₂ COMPOSITE ELECTRODE AND MECHANISM OF CATALYTIC OXIDATION OF BISPHENOL A

1. State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China;
2. National Engineering Research Center for Urban Pollution Control, Tongji University, Shanghai 200092, China;
3. Hebei Construction Group Installation Engineering Co., Ltd, Baoding 071000, China

摘要

摘要: 采用电化学沉积法将不同浓度的碳纳米管（CNT）掺入PbO₂电极，得到具有高稳定性和催化活性的CNT-PbO₂复合电极。扫描电子显微镜（SEM）、能量色散谱（EDS）等测试分析发现CNT掺杂到PbO₂电极表面活性层中，CNT掺杂使得PbO₂晶粒尺寸减小，活性表面积增大。CNT-PbO₂电极降解双酚A体系中自由基生成量减少，但其降解效果反而提升。循环伏安测试（CV）、电极加速寿命测试表明，CNT-PbO₂电极降解双酚A的机理主要是改性后的电极具有更强的电化学直接氧化能力和更高的稳定性。最后通过UPLC&Q-TOF MS测试得到双酚A的主要降解产物和降解路径。
- 碳纳米管 /
- 改性PbO₂电极 /
- 电催化氧化 /
- 双酚A /
- 降解机理
Abstract: CNT-PbO₂ composite electrodes with high stability and catalytic activity were obtained by doping carbon nanotubes (CNTs) with different concentrations into PbO₂ electrodes by electrochemical deposition. Scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS) analysis proved that CNTs were successfully doped into the PbO₂ electrode surface active layer, leading to a decline of PbO₂ particle size and an increase of activity surface area. The amount of ·OH radicals generated in the degradation system of bisphenol A (BPA) by CNT-PbO₂ electrodes decreased. However, the degradation effect was improved. Cyclic voltammetry (CV) curves and the accelerated life test indicated that the degradation mechanism of BPA was mainly ascribed to the stronger electrochemical direct oxidation ability and higher stability of CNT-PbO₂ composite electrodes. Finally, the dominant by-products were obtained, and plausible degradation pathway of BPA was proposed by UPLC & Q-TOF MS test.
- carbon nanotubes /
- modified PbO₂ electrodes /
- electrocatalytic oxidation /
- bisphenol A /
- degradation mechanism

HTML全文

参考文献(16)

[1]	ZHU X P, NI J R, LAI P. Advanced treatment of biologically pretreated coking wastewater by electrochemical oxidation using boron-doped diamond electrodes[J]. Water Research, 2009, 43(17):4347-4355.
[2]	WEI J Z, FENG Y J, SUN X J, et al. Effectiveness and pathways of electrochemical degradation of pretilachlor herbicides[J]. Journal of Hazardous Materials, 2011, 189(1/2):84-91.
[3]	PANIZZA M, CERISOLA G. Influence of anode material on the electrochemical oxidation of 2-naphthol:Part 1. Cyclic voltammetry and potential step experiments[J]. Electrochimica Acta, 2003, 48(23):3491-3497.
[4]	ZHANG C, LIU J H, CHEN B M. Effect of CeO₂ and graphite powder on the electrochemical performance of Ti/PbO₂ anode for zinc electrowinning[J]. Ceramics International, 2018, 44(16):19735-19742.
[5]	AMADELLI R, SAMIOLO L, VELICHENKO A B, et al. Composite PbO₂-TiO₂ materials deposited from colloidal electrolyte:electrosynthesis, and physicochemical properties[J]. Electrochimica Acta, 2009, 54(22):5239-5245.
[6]	ZHANG S, QUAN X, ZHENG J F, et al. Probing the interphase "HO zone" originated by carbon nanotube during catalytic ozonation[J]. Water Research, 2017, 122:86-95.
[7]	DUAN X Y, MA F, YUAN Z X, et al. Lauryl benzene sulfonic acid sodium-carbon nanotube-modified PbO₂ electrode for the degradation of 4-chlorophenol[J]. Electrochimica Acta, 2012, 76:333-343.
[8]	CHANG L M, ZHOU Y, DUAN X Y, et al. Preparation and characterization of carbon nanotube and Bi co-doped PbO₂ electrode[J]. Journal of the Taiwan Institute of Chemical Engineers, 2014, 45(4):1338-1346.
[9]	段小月. 碳纳米管改性PbO₂电极制备及降解水中酚类污染物的研究[D]. 哈尔滨:哈尔滨工业大学, 2013.
[10]	DAI Q Z, XIA Y J, CHEN J M. Mechanism of enhanced electrochemical degradation of highly concentrated aspirin wastewater using a rare earth La-Y co-doped PbO₂ electrode[J]. Electrochimica Acta, 2016, 188:871-881.
[11]	XU F, CHANG L M, DUAN X Y, et al. A novel layer-by-layer CNT/PbO₂ anode for high-efficiency removal of PCP-Na through combining adsorption/electrosorption and electrocatalysis[J]. Electrochimica Acta, 2019, 300:53-66.
[12]	YANG C J, SHEN Q F, ZHAI D C, et al. Carbon nanotubes sheathed in lead for the oxygen evolution in zinc electrowinning[J]. Journal of Applied Electrochemistry, 2019, 49(1):67-77.
[13]	GILROY D. The breakdown of PbO₂-Ti anodes[J]. Journal of Applied Electrochemistry, 1982, 12(2):171-183.
[14]	罗瑶, 薛娟琴, 于丽花, 等. 不同咪唑基离子液体改性PbO₂电极降解苯酚废水[J]. 环境工程学报, 2017, 11(5):2671-2676.
[15]	ZHAN M J, YANG X, XIAN Q M, et al. Photosensitized degradation of bisphenol A involving reactive oxygen species in the presence of humic substances[J]. Chemosphere, 2006, 63(3):378-386.
[16]	POERSCHMANN J, TROMMLER U, GÓRECKI T. Aromatic intermediate formation during oxidative degradation of Bisphenol A by homogeneous sub-stoichiometric Fenton reaction[J]. Chemosphere, 2010, 79(10):975-986.