Effective degradation of ibuprofen by flow-through electro-peroxone process
CUI Xin-xin1, LIN Zhi-rong2, WANG Hui-jiao1, YU Gang1, WANG Yu-jue1
1. School of Environment, Tsinghua University, Beijing 100084, China;
2. Collage of Geographical and Environmental Engineering, Gannan Normal University, Ganzhou 341000, China
By combining conventional ozonation with in situ electro-generation of hydrogen peroxide (H2O2) to enhance ozone (O3) transformation to hydroxyl radicals (·OH), the electro-peroxone (E-peroxone) treatment can significantly enhance the oxidation of ozone-refractory pollutants. A flow-through E-peroxone system was established using a reticulated vitreous carbon (RVC) as the cathode. The effects of main operational parameters (e.g., current and flow rate) on ibuprofen abatement were evaluated systematically. The results showed that the E-peroxone process could completely abate ibuprofen (initial concentration 2.5mg/L) in a synthetic solution in 30min, whereas conventional ozonation and electrolysis could only abated 64% and 59% of ibuprofen, respectively. The electrical energy consumption per log-order removal (EEO, kWh/m3-log) of ibuprofen by ozonation was 5.30kWh/m3-log, but was only 0.76kWh/m3-log by the E-peroxone process under the conditions of 100mA, 250mL/min gas flow rate, 8mg/L ozone and 300mL/min solution flow rate. Increasing the solution flow rate to increase the kinetics of electrode mass transfer, the rate of ibuprofen abatement could be further enhanced in the flow-through E-peroxone process. These results suggest that flow-through E-peroxone process may provide an effective and energy-efficient alternative for the abatement of refractory pollutants in water treatment.
崔欣欣, 林志荣, 王会姣, 余刚, 王玉珏. 基于穿透电极的Electro-peroxone技术降解布洛芬[J]. 中国环境科学, 2019, 39(4): 1619-1626.
CUI Xin-xin, LIN Zhi-rong, WANG Hui-jiao, YU Gang, WANG Yu-jue. Effective degradation of ibuprofen by flow-through electro-peroxone process. CHINA ENVIRONMENTAL SCIENCECE, 2019, 39(4): 1619-1626.
Daughton C G, Ternes T A. Pharmaceuticals and personal care products in the environment:agents of subtle change[J]. Environmental Health Perspectives, 1999,107(Suppl 6):907-938.
[2]
Esplugas S, Bila D M, Krause L G, et al. Ozonation and advanced oxidation technologies to remove endocrine disrupting chemicals (EDCs) and pharmaceuticals and personal care products (PPCPs) in water effluents[J]. Journal of Hazardous Materials, 2007,149(3):631-642.
[3]
Carballa M, Omil F, Lema J M, et al. Behavior of pharmaceuticals, cosmetics and hormones in a sewage treatment plant[J]. Water Research, 2004,38(12):2918-2926.
[4]
Oller I, Malato S, Sánchez-Pérez J A. Combination of Advanced Oxidation Processes and biological treatments for wastewater decontamination——a review[J]. Energy Environmental Protection, 2012,409(20):4141-4166.
[5]
赵琦,何小娟,唐翀鹏,等.药物和个人护理用品(PPCPs)处理方法研究进展[J]. 净水技术, 2010,29(4):5-10. Zhao Q, He X, Tang C, et al. Research progress on treatment processes of pharmaceuticals and personal care products (PPCPs)[J]. Water Purification Technology, 2010,29(4):5-10.
[6]
Rossner A, Snyder S A, Knappe D R U. Removal of emerging contaminants of concern by alternative adsorbents[J]. Water Research, 2009,43(15):3787-3796.
[7]
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.
[8]
Wang Y, Li X, Zhen L, et al. Electro-Fenton treatment of concentrates generated in nanofiltration of biologically pretreated landfill leachate[J]. Journal of Hazardous Materials, 2012,229-230(3):115-121.
[9]
袁实.电催化臭氧水处理技术的开发和研究[D]. 北京:清华大学, 2014. Yuan S. The development of a novel Electro-peroxone technology for water and wastewater treatment[D]. Beijing:Tsinghua University, 2014.
[10]
Klavarioti M, Mantzavinos D, Kassinos D. Removal of residual pharmaceuticals from aqueous systems by advanced oxidation processes[J]. Environment International, 2009,35(2):402-417.
[11]
Matilainen A, Sillanpää M. Removal of natural organic matter from drinking water by advanced oxidation processes[J]. Chemosphere, 2010,80(4):351-365.
[12]
Huber M M, Canonica S, Gunyoung Park A, et al. Oxidation of pharmaceuticals during ozonation and advanced oxidation processes[J]. Environmental Science & Technology, 2003,37(5):1016-24.
[13]
Sirés I, Brillas E. Remediation of water pollution caused by pharmaceutical residues based on electrochemical separation and degradation technologies:a review[J]. Environment International, 2012,40(40):212-229.
[14]
Panizza M, Cerisola G. Direct and mediated anodic oxidation of organic pollutants[J]. Chemical Reviews, 2009,109(12):6541.
[15]
Moreira F C, Soler J, Fonseca A, et al. Electrochemical advanced oxidation processes for sanitary landfill leachate remediation:Evaluation of operational variables[J]. Applied Catalysis B Environmental, 2016,182:161-171.
[16]
Ji Y, Wang J, Jia J P. Improvement of electrochemical wastewater treatment through mass transfer in a seepage carbon nanotube electrode reactor[J]. Environmental Science & Technology, 2009, 43(10):3796-802.
[17]
Rosal R, Rodríguez A, Perdigónmelón J A, et al. Removal of pharmaceuticals and kinetics of mineralization by O3/H2O2 in a biotreated municipal wastewater[J]. Water Research, 2008,42(14):3719-3728.
[18]
Lee Y, Gerrity D, Lee M, et al. Prediction of micropollutant elimination during ozonation of municipal wastewater effluents:use of kinetic and water specific information[J]. Environmental Science & Technology, 2013,47(11):5872-5881.
[19]
Lee Y, Kovalova L, Mcardell C S, et al. Prediction of micropollutant elimination during ozonation of a hospital wastewater effluent[J]. Environmental Science & Technology, 2013,47(11):5872-5881.
[20]
Quero-Pastor M J, Garrido-Perez M C, Acevedo A, et al. Ozonation of ibuprofen:a degradation and toxicity study[J]. Science of the Total Environment, 2014,466-467(1):957-964.
[21]
Tekle-Röttering A, Jewell K S, Reisz E, et al. Ozonation of piperidine, piperazine and morpholine:Kinetics, stoichiometry, product formation and mechanistic considerations[J]. Water Research, 2016,88(2):960-971.
[22]
李启彬,张爱平,李民,等.O3/H2O2降解垃圾渗滤液浓缩液的氧化特性及光谱解析[J]. 中国环境科学, 2017,37(6):2160-2172. Chen W, Zhang A, Li M, et al. Decomposition of organics in concentrated landfill leachate with ozone/hydrogen peroxide system:Oxidation characteristics and spectroscopic analyses[J]. China Environmental Science, 2017,37(6):2160-2172.
[23]
Li X, Wang Y, Yuan S, et al. Degradation of the anti-inflammatory drug ibuprofen by electro-peroxone process[J]. Water Research, 2014, 63(7):81-93.
[24]
Bakheet B, Yuan S, Li Z, et al. Electro-peroxone treatment of Orange Ⅱ dye wastewater[J]. Water Research, 2013,47(16):6234-6243.
[25]
Yuan S, Li Z, Wang Y. Effective degradation of methylene blue by a novel electrochemically driven process[J]. Electrochemistry Communications, 2013,29(10):48-51.
[26]
Qiu C, Yuan S, Li X, et al. Investigation of the synergistic effects for p-nitrophenol mineralization by a combined process of ozonation and electrolysis using a boron-doped diamond anode[J]. Journal of Hazardous Materials, 2014,280(280C):644-653.
[27]
Li Z, Yuan S, Qiu C, et al. Effective degradation of refractory organic pollutants in landfill leachate by electro-peroxone treatment[J]. Electrochimica Acta, 2013,102(21):174-182.
[28]
Frangos P, Wang H, Shen W, et al. A novel photoelectro-peroxone process for the degradation and mineralization of substituted benzenes in water[J]. Chemical Engineering Journal, 2016,286:239-248.
[29]
Wang H, Yuan S, Zhan J, et al. Mechanisms of enhanced total organic carbon elimination from oxalic acid solutions by electro-peroxone process[J]. Water Research, 2015,80:20-29.
[30]
Li Y, Shen W, Fu S, et al. Inhibition of bromate formation during drinking water treatment by adapting ozonation to electro-peroxone process[J]. Chemical Engineering Journal, 2015,264:322-328.
[31]
Bakheet B, Qiu C, Yuan S, et al. Inhibition of polymer formation in electrochemical degradation of p-nitrophenol by combining electrolysis with ozonation[J]. Chemical Engineering Journal, 2014, 252(5):17-21.
[32]
Wang H, Bakheet B, Yuan S, et al. Kinetics and energy efficiency for the degradation of 1,4-dioxane by electro-peroxone process[J]. Journal of Hazardous Materials, 2015,294:90-98.
[33]
Yao W, Wang X, Yang H, et al. Removal of pharmaceuticals from secondary effluents by an electro-peroxone process[J]. Water Research, 2016,88:826-835.
[34]
Gonzálezgarcía J, Bonete P, Expósito E, et al. Characterization of a carbon felt electrode:structural and physical properties[J]. Journal of Materials Chemistry, 1999,9(2):419-426.
[35]
Gonzálezgarcía J, Vicente Montiel A, Aldaz A, et al. Hydrodynamic behavior of a filter-press electrochemical reactor with carbon felt as a three-dimensional electrode[J]. Industrial & Engineering Chemistry Research, 1998,37(11):4501-4511.
[36]
Liu Y, Liu H, Zhou Z, et al. Degradation of the common aqueous antibiotic tetracycline using a carbon nanotube electrochemical filter[J]. Environmental Science & Technology, 2015,49(13):7974-80.
[37]
Gao G, Pan M, Vecitis C D. Effect of oxidation approach on carbon nanotube surface functional groups and electrooxidative filtration performance[J]. Journal of Materials Chemistry A, 2015,3(14):7575-7582.
[38]
Yue Z R, Jiang W, Wang L, et al. Surface characterization of electrochemically oxidized carbon fibers[J]. Carbon, 1999,37(11):1785-1796.
[39]
Gao G, Zhang Q, Hao Z, et al. Carbon nanotube membrane stack for flow-through sequential regenerative electro-Fenton[J]. Environmental Science & Technology, 2015,49(4):2375.
[40]
Friedrich J M, Ponce-De-León C, Reade G W, et al. Reticulated vitreous carbon as an electrode material[J]. Journal of Electroanalytical Chemistry, 2004,561(1/2):203-217.
[41]
Kuo C H, Li Z, Zappi M E, et al. Kinetics and mechanism of the reaction between ozone and hydrogen peroxide in aqueous solutions[J]. Canadian Journal of Chemical Engineering, 2010,77(3):473-482.
[42]
Zhou W, Gao J, Ding Y, et al. Drastic enhancement of H2O2 electrogeneration by pulsed current for Ibuprofen degradation:strategy based on decoupling study on H2O2 decomposition pathways[J]. Chemical Engineering Journal, 2017,338:709-718.
[43]
Liu H, Vecitis C D. Reactive transport mechanism for organic oxidation during electrochemical filtration:Mass-transfer, physical adsorption, and electron-transfer[J]. Journal of Physical Chemistry C, 2016,116(1):374-383.
[44]
Ambuludi, Loaiza S, Oturan, et al. Kinetic behavior of antiinflammatory drug ibuprofen in aqueous medium; during its degradation by electrochemical advanced oxidation[J]. Environmental Science & Pollution Research International, 2013,20(4):2381-2389.
[45]
Bolton J R, Bircher K G, Tumas W, et al. Figures-of-merit for the technical development and application of advanced oxidation technologies for both electric-and solar-driven systems (IUPAC Technical Report)[J]. Pure & Applied Chemistry, 2001,73(4):627-637.
[46]
杨丽娟,胡翔,吴晓楠.Fenton法降解水中布洛芬[J]. 环境化学, 2012,31(12):1896-1900. Yang L, Hu X, Wu X. Degradation of ibuprofen by Fenton oxidation[J]. Environmental Chemistry, 2012,31(12):1896-1900.
[47]
朱宏,胡翔.铁炭微电解法降解布洛芬的研究[J]. 环境工程学报, 2013,7(5):1735-1738. Zhu H, Hu X. Study on degradation of ibuprofen by iron-carbon micro-electrolysis[J]. Chinese Journal of Environmental Engineering, 2013,7(5):1735-1738.
[48]
苏海英,王盈霏,王枫亮,等.g-C3N4/TiO2复合材料光催化降解布洛芬的机制[J]. 中国环境科学, 2017,37(1):195-202. Su H, Wang Y, Wang F, et al. Preparation of g-C3N4/TiO2 composites and the mechanism research of the photocatalysis degradation of ibuprofen[J]. China Environmental Science, 2017,37(1):195-202.
[49]
汤迎,虢清伟,洪澄泱,等.活性污泥去除4种典型药品的研究[J]. 工业水处理, 2016,36(2):63-66. Tang Y, Guo Q, Hong C, et al. Research on the removal of four kinds of typical medicine by activated sludge[J]. Industrial Water Treatment, 2016,36(2):63-66.
