Enhancement of H2O2 accumulationat gas diffusion electrodes (GDEs) optimized by 3D-printed technique and its utilization in electro-Fenton for coking wastewater treatment
QIU Shan1,2, GAO Wei-jie1,2, DENG Feng-xia1,2, ZHU Ying-shi1,2, MA Fang1,2, YANG Ji-xian1,2
1. School of Environment, Harbin Institute of Technology, Harbin 150090, China;
2. State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin 150090, China
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.
邱珊, 高伟杰, 邓凤霞, 朱英实, 马放, 杨基先. 3D打印气体扩散电极产H2O2及其对焦化废水的处理研究[J]. 中国环境科学, 2018, 38(11): 4075-4084.
QIU Shan, GAO Wei-jie, DENG Feng-xia, ZHU Ying-shi, MA Fang, YANG Ji-xian. Enhancement of H2O2 accumulationat gas diffusion electrodes (GDEs) optimized by 3D-printed technique and its utilization in electro-Fenton for coking wastewater treatment. CHINA ENVIRONMENTAL SCIENCECE, 2018, 38(11): 4075-4084.
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.
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.
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.
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.
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.
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.