3D打印气体扩散电极产H<sub>2</sub>O<sub>2</sub>及其对焦化废水的处理研究

Abstract
Figure/Table
References (40)
Related Citation (15)

Download: PDF (670 KB) HTML (1 KB)
Export: BibTeX | EndNote (RIS)

Abstract

In this study, 3D-printed GDE (3D-GDE) with a high H₂O₂ generation rate was designed using a three-dimensional printing approach and its application in electro-Fenton for coking wastewater treatment. Results showed that H₂O₂ reached 16.1mg H₂O₂/cm², which was superior to the conventional gas diffusion electrode in the absence of the 3D-printedstructure with 7.16mg H₂O₂/cm² H₂O₂ capacity under the same conditions. Moreover, it showed acid condition was favorable for the H₂O₂ production, and H₂O₂ generation rose from 250mg/L to 450mg/L as current increased from 200mA to 250mA. However, a further enhancement in current failed to improve H₂O₂ generation capacity. The proposed system was used for coking wastewater treatment following the optimization of the operating factors. Mineralization rate of coking wastewater could reach as high as 80% in 4h electrolysis by the 3D-GDE electro-Fenton process. Moreover, three-dimensional fluorescence method confirmed the effectiveness of the process in a direct approach. Microtox toxicity results revealed that the 3D-GDE electro-Fenton process was effective for coking wastewater detoxification and the lowest energy consumption for coking wastewater was calculated as 0.9kW·h/g TOC.

Key words： 3D-printed technique gas diffusion electrodes (GDEs) electro-fenton (EF) phenol coking wastewater Microtox

Received: 10 April 2018

X703

	Service

	E-mail this article
	Add to my bookshelf
	Add to citation manager
	E-mail Alert
	RSS
	Articles by authors
	QIU Shan
	GAO Wei-jie
	DENG Feng-xia
	ZHU Ying-shi
	MA Fang
	YANG Ji-xian

Cite this article:

QIU Shan,GAO Wei-jie,DENG Feng-xia等. Enhancement of H₂O₂ accumulationat gas diffusion electrodes (GDEs) optimized by 3D-printed technique and its utilization in electro-Fenton for coking wastewater treatment[J]. CHINA ENVIRONMENTAL SCIENCECE, 2018, 38(11): 4075-4084.

URL:

http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2018/V38/I11/4075

[1]	WANG C, ZHANG M, LIU W, et al. Effluent characteristics of advanced treatment for biotreated coking wastewater by electrochemical technology using BDD anodes[J]. Environmental Science & Pollution Research International, 2015,22(9):6827-6834.
[2]	张锦,李圭白,马军.含酚废水的危害及处理方法的应用特点[J]. 化学工程师, 2001,(2):36-37.
[3]	MARTÍNEZ-HUITLE C A, RODRIGO M A, SIRÉS I, et al. Single and coupled electrochemical processes and reactors for the abatement of organic water pollutants:a critical review[J]. Chemical Reviews, 2015,115(24):13362-13407.
[4]	QIU S, HE D, MA J, et al. Kinetic modeling of the electro-Fenton process:quantification of reactive oxygen species generation[J]. Electrochimica Acta, 2015,176:51-58.
[5]	SIRÉS I, BRILLAS E, OTURAN M A, et al. Electrochemical advanced oxidation processes:today and tomorrow. A review[J]. Environmental Science and Pollution Research, 2014,21(14):8336-8367.
[6]	BRILLAS E, SIRES I, OTURAN M A. Electro-Fenton process and related electrochemical technologies based on Fenton's reaction chemistry[J]. Chemical reviews, 2009,109(12):6570-6631.
[7]	YANG K S, MUL G, MOULIJN J A. Electrochemical generation of hydrogen peroxide using surface area-enhanced Ti-mesh electrodes[J]. Electrochimica acta, 2007,52(22):6304-6309.
[8]	LEI H, LI H, LI Z, et al. Electro-Fenton degradation of cationic red X-GRL using an activated carbon fiber cathode[J]. Process safety and environmental protection, 2010,88(6):431-438.
[9]	LIU X, YANG D, ZHOU Y, et al. Electrocatalytic properties of N-doped graphite felt in electro-Fenton process and degradation mechanism of levofloxacin[J]. Chemosphere, 2017,182:306-315.
[10]	SANDU C, POPESCU M, ROSALES E, et al. Electrokinetic oxidant soil flushing:A solution for in situ remediation of hydrocarbons polluted soils[J]. Journal of Electroanalytical Chemistry, 2017,799:1-8.
[11]	CHEN W, YANG X, HUANG J, et al. Iron oxide containing graphene/carbon nanotube based carbon aerogel as an efficient E-Fenton cathode for the degradation of methyl blue[J]. Electrochimica Acta, 2016,200:75-83.
[12]	SOLANO A M S, MARTÍNEZ-HUITLE C A, GARCIA-SEGURA S, et al. Application of electrochemical advanced oxidation processes with a boron-doped diamond anode to degrade acidic solutions of Reactive Blue 15(Turqueoise Blue) dye[J]. Electrochimica Acta, 2016,197:210-220.
[13]	BANUELOS J A, EI-GHENYMY A, RODRIGUEZ F J, et al. Study of an air diffusion activated carbon packed electrode for an electro-Fenton wastewater treatment[J]. Electrochimica Acta, 2014,140(SI):412-418.
[14]	王雪莹.3D打印技术与产业的发展及前景分析[J]. 中国高新技术企业, 2012,(26):3-5.
[15]	李小丽,马剑雄,李萍,等.3D打印技术及应用趋势[J]. 自动化仪表, 2014,(1):1-5.
[16]	BRILLAS E, LLOSA E, CASADO J, et al. Electrochemical destruction of aniline and 4-chloroaniline for wastewater treatment using a carbon-PTFE O2-fed-cathode[J]. Journal of the Electrochemical Society, 1995,142(6):1733-1741.
[17]	JUNGLEE S, URBAN L, SALLANON H, et al. Optimized assay for hydrogen peroxide determination in plant tissue using potassium iodide[J]. American Journal of Analytical Chemistry, 2014,5:730-736.
[18]	MOUSSET E, KO Z T, SYAFIQ M, et al. Electrocatalytic activity enhancement of a graphene ink-coated carbon cloth cathode for oxidative treatment[J]. Electrochimica Acta, 2016,222:1628-1641.
[19]	肖华,周荣丰.电芬顿法的研究现状与发展[J]. 上海环境科学, 2004,(6):253-256.
[20]	张锋.电芬顿法降解苯酚废水的研究[J]. 广州化工, 2014, (10):116-117.
[21]	毕强,薛娟琴,郭莹娟,等.电芬顿法去除兰炭废水COD[J]. 环境工程学报, 2012,(12):4310-4314.
[22]	POZZO A D, PALMA L D, MERLI C, et al. An experimental comparison of a graphite electrode and a gas diffusion electrode for the cathodic production of hydrogen peroxide[J]. Journal of Applied Electrochemistry, 2005,35(4):413-419.
[23]	YU X, ZHOU M, REN G, et al. A novel dual gas diffusion electrodes system for efficient hydrogen peroxide generation used in electro-Fenton[J]. Chemical Engineering Journal, 2015,263:92-100.
[24]	邱珊,柴一荻,古振澳,等.电芬顿反应原理研究进展[J]. 环境科学与管理, 2014,(9):55-58.
[25]	XIA G, LU Y, XU H. Electrogeneration of hydrogen peroxide for electro-Fenton via oxygen reduction using polyacrylonitrile-based carbon fiber brush cathode[J]. Electrochimica Acta, 2015,158:390-396.
[26]	郁青红,周明华,雷乐成.新型气体扩散电极体系高效产H2O2的研究[J]. 物理化学学报, 2006,(7):883-887.
[27]	汤培.石墨/聚四氟乙烯气体扩散电极的制备及其性能研究[D]. 河北:燕山大学, 2012.
[28]	VALIM R B, REIS R M, CASTRO P S, et al. Electrogeneration of hydrogen peroxide in gas diffusion electrodes modified with tert-butyl-anthraquinone on carbon black support[J]. Carbon, 2013,61:236-244.
[29]	GARCÍA-RODRÍGUEZ O, BAÑUELOS J A, EL-GHENYMY A, et al. Use of a carbon felt-iron oxide air-diffusion cathode for the mineralization of Malachite Green dye by heterogeneous electro-Fenton and UVA photoelectro-Fenton processes[J]. Journal of Electroanalytical Chemistry, 2016,767:40-48.
[30]	ZHANG Z, MENG H, WANG Y, et al. Fabrication of graphene@graphite-based gas diffusion electrode for improving H2O2 generation in electro-Fenton process[J]. Electrochimica Acta, 2018, 260:112-120.
[31]	LIU T, WANG K, SONG S, et al. New electro-Fenton gas diffusion cathode based on nitrogen-doped graphene@carbon nanotube composite materials[J]. Electrochimica Acta, 2016,194(Supplement C):228-238.
[32]	CHEN Z, DONG H, YU H, et al. In-situ electrochemical flue gas desulfurization via carbon black-based gas diffusion electrodes:performance, kinetics and mechanism[J]. Chemical Engineering Journal, 2017,307:553-561.
[33]	BANUELOS J A, EI-GHENYMY A, RODRIGUEZ F J, et al. Study of an air diffusion activated carbon packed electrode for an electro-Fenton wastewater treatment[J]. Electrochimica Acta, 2014,140(SI):412-418.
[34]	FORTI J C, VENANCIO C E, LANZA M R V, et al. Effects of the modification of gas diffusion electrodes by organic redox catalysts for hydrogen peroxide electrosynthesis[J]. Journal of The Brazilian Chemical Society, 2008,19(4):643-650.
[35]	BRILLAS E, SIRÉS I, OTURAN M A. Electro-Fenton process and related electrochemical technologies based on Fenton's reaction chemistry.[J]. Chemical Reviews, 2009,109(12):6570-6631.
[36]	PIMENTEL M, OTURAN N, DEZOTTI M, et al. Phenol degradation by advanced electrochemical oxidation process electro-Fenton using a carbon felt cathode[J]. Applied Catalysis B:Environmental, 2008, 83(1):140-149.
[37]	ALARCÓN F, BÁEZ M E, BRAVO M, et al. Feasibility of the determination of polycyclic aromatic hydrocarbons in edible oils via unfolded partial least-squares/residual bilinearization and parallel factor analysis of fluorescence excitation emission matrices[J]. Talanta, 2013,103(21):361.
[38]	ARIESE F, ASSEMA S V, GOOIJER C, et al. Comparison of laurentian fulvic acid luminescence with that of the hydroquinone/quinone model system:evidence from low temperature fluorescence studies and EPR spectroscopy[J]. Aquatic Sciences, 2004,66(1):86-94.
[39]	LI J, LIU X, WANG S, et al. Synthesis and optimization of a novel poly-silicic metal coagulant from coal gangue for tertiary-treatment of coking wastewater[J]. Journal of Chemical Technology & Biotechnology, 2017.
[40]	BARHOUMI N, OTURAN N, OLVERA-VARGAS H, et al. Pyrite as a sustainable catalyst in electro-Fenton process for improving oxidation of sulfamethazine. Kinetics, mechanism and toxicity assessment[J]. Water Research, 2016,94:52-61.