外加电流阴极保护强化ACF激活PDS降解水中卡马西平
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摘要
卡马西平是一种典型的持久性的有机药物污染物,采用一种新的外加电流阴极保护强化活性炭纤维(ACF)激活过硫酸盐(PDS)的高级氧化方法,实现对水中卡马西平的高效降解.考察该体系对比活性炭纤维激发过硫酸盐体系、阴极保护活性炭纤维电解体系、过硫酸盐体系、活性炭纤维吸附体系、电解体系等不同工艺对卡马西平的降解率,探究过硫酸盐初始浓度、电压、初始pH等因素对体系的影响,并通过活性炭纤维性质测定和自由基捕获探究其降解机制.结果显示,外加电流阴极保护增强活性炭纤维(ACF)激活过硫酸盐(PDS)体系对水中卡马西平的氧化降解率远高于其他5种处理工艺.在外加电流阴极保护强化活性炭纤维(ACF)激活过硫酸盐(PDS)体系中,过高的过硫酸盐浓度反而不利于卡马西平的降解,在一定条件下存在一个适宜的过硫酸盐浓度范围;电压的提高和初始pH为酸性(pH=3)更有利于对卡马西平的氧化降解.此外,该体系中活性炭纤维受到阴极电场保护,使用寿命大大延长.硫酸根自由基在体系去除卡马西平过程中起主导作用.
A novel oxidation way of electrically protected and enhanced activated carbon fibers( ACF) activating peroxodisulfate( PDS) was adopted in this work for the degradation of aqueous Carbamazepine,a sort of typical persistent medical pollutant. The removal rate by PDS system,ACF adsorption system,ACF activating PDS system,electrolysis system,protected ACF electrolysis system,and electrically protected and enhanced ACF activating PDS system was studied. The influences of PDS initial concentration,voltage,and initial pH value on the degradation of carbamazepine were also researched. Besides,characteristics detection of activated carbon fibers and radical quenching were conducted to reveal the oxidation mechanism in electrically protected and enhanced ACF activating PDS system. The results showed that the removal rate of carbamazepine in electrically protected and enhanced ACF activating PDS system was much higher than that in other processes. The excessive high initial PDS concentration could not promote the removal rate of carbamazepine. The removal rate of carbamazepine increased with the increase of voltage and the decrease of initial pH value. Activated carbon fibers could be protected from oxidation damaging with free electron implantation in cathode in electrically protected and enhanced ACF activating PDS process,which greatly prolonged its service life and significantly improved the utilization rate of PDS.
A novel oxidation way of electrically protected and enhanced activated carbon fibers( ACF) activating peroxodisulfate( PDS) was adopted in this work for the degradation of aqueous Carbamazepine,a sort of typical persistent medical pollutant. The removal rate by PDS system,ACF adsorption system,ACF activating PDS system,electrolysis system,protected ACF electrolysis system,and electrically protected and enhanced ACF activating PDS system was studied. The influences of PDS initial concentration,voltage,and initial pH value on the degradation of carbamazepine were also researched. Besides,characteristics detection of activated carbon fibers and radical quenching were conducted to reveal the oxidation mechanism in electrically protected and enhanced ACF activating PDS system. The results showed that the removal rate of carbamazepine in electrically protected and enhanced ACF activating PDS system was much higher than that in other processes. The excessive high initial PDS concentration could not promote the removal rate of carbamazepine. The removal rate of carbamazepine increased with the increase of voltage and the decrease of initial pH value. Activated carbon fibers could be protected from oxidation damaging with free electron implantation in cathode in electrically protected and enhanced ACF activating PDS process,which greatly prolonged its service life and significantly improved the utilization rate of PDS.
引文
[1]KOSJEK T,ANDERSEN H R,KOMPARE B,et al. Fate of carbamazepine during water treatment[J]. Environmental Science&Technology,2009,43(16):6256
[2]SCHEYTT T,MERSMANN P,LINDSTADT R,et al. Determination of sorption coefficients of pharmaceutically active substances carbamazepine,diclofenac,and ibuprofen,in sandy sediments[J].Chemosphere,2005,60(2):245
[3] ZHANG Yuqing, GEISSEN S, GAL C. Carbamazepine and diclofenac:Removal in wastewater treatment plants and occurrence in water bodies[J]. Chemosphere,2008,73(8):1151
[4]TERNES T A. Occurrence of drugs in German sewage treatment plants and rivers[J]. Water Research,1998,32(11):3245
[5]PAXEUS N. Removal of selected non-steroidal anti-inflammatory drugs(NSAIDs), gemfibrozil, carbamazepine, beta-blockers,trimethoprim and triclosan in conventional wastewater treatment plants in five EU countries and their discharge to the aquatic environment[J]. Water Science&Technology A Journal of the International Association on Water Pollution Research,2004,50(5):253. DOI:10. 2166/wst. 2004. 0335
[6]陈晓旸,薛智勇,吴丹,等.基于硫酸自由基的高级氧化技术及其在水处理中的应用[J].水处理技术,2009,35(5):16CHEN Xiaoyang, XUE Zhiyong, WU Dan, et al. Advanced oxidation technology based on sulfuric acid free radicals and its application in water treatment[J]. Technology Water Treatment,2009,35(5):16. DOI:10. 16796/j. cnki. 1000-3770. 2009. 05.005
[7]MATTA R,TLILI S,CHIRON S,et al. Removal of carbamazepine from urban wastewater by sulfate radical oxidation[J].Environmental Chemistry Letters,2011,9(3):347
[8]OLMEZ-HANCI T,ARSLAN-ALATON I. Comparison of sulfate and hydroxyl radical based advanced oxidation of phenol[J]. Chemical Engineering Journal,2013,224(1):10
[9]马京帅,吕文英,刘国光,等.吉非罗齐在热活化过硫酸盐体系中的降解机制研究[J].环境科学学报,2016,36(10):3774MA Jingshuai,LV Wenying,LIU Guoguang,et al. Degradation mechanism of gemfibrozil in heat-activated persulfate oxidation process[J]. Acta Scientiae Circumstantiae,2016,36(10):3774.DOI:10. 13671/j. hjkxxb. 2016. 0064
[10]SHU Hungyee,CHANG Mingchin,HUANG Shiwei. UV irradiation catalyzed persulfate advanced oxidation process for decolorization of Acid Blue 113 wastewater[J]. Desalination and Water Treatment,2015,54(4/5):1013
[11]高金龙,马玉琳,孟庆来,等.二价铁活化过硫酸盐降解土壤中十溴联苯醚[J].环境工程学报,2016(12):7339GAO Jinlong,MA Yulin,MENG Qinglai,et al. Degradation of decabromodiphenyl ether in soil by sulfate activated with ferrous ions[J]. Chinese Journal of Environmental Engineering,2016(12):7339. DOI:10. 12030/j. cjee. 201507210
[12]TEEL A L,AHMAD M,WATTS R J. Persulfate activation by naturally occurring trace minerals[J]. Journal of Hazardous Materials,2011,196(1):153
[13]QI Chengdu,LIU Xitao,LIN Chunye,et al. Degradation of sulfamethoxazole by microwave-activated persulfate:Kinetics,mechanism and acute toxicity[J]. Chemical Engineering Journal,2014,249:6
[14]SAPUTRA E,MUHAMMAD S,SUN H,et al. Activated carbons as green and effective catalysts for generation of reactive radicals in degradation of aqueous phenol[J]. RSC Advances,2013,3(44):21905
[15]施周,毕晨,周石庆,等.铁电极活化过硫酸盐对金橙G的降解[J].环境工程学报,2017,11(3):1335SHI Zhou,BI Chen,ZHOU Shiqing,et al. Degradation of iron electrode as sodium persulfate activator for orange G[J]. Chinese Journal of Environmental Engineering,2017,11(3):1335. DOI:10. 12030/j. cjee. 201511172
[16]YANG Shiying,YANG Xin,SHAO Xueting,et al. Activated carbon catalyzed persulfate oxidation of Azo dye acid orange 7 at ambient temperature[J]. Journal of Hazardous Materials,2011,186(1):659
[17]SANCHEZ-POLO M,VON G U,RIVERA-UTRILLA J. Efficiency of activated carbon to transform ozone into*OH radicals:Influence of operational parameters[J]. Water Research,2005,39(14):3189
[18]FARIA P C C,ORFAO J J M,PEREIRA M F R. Ozone decomposition in water catalyzed by activated carbon:Influence of chemical and textural properties[J]. Industrial&Engineering Chemistry Research, 2006, 45(8):2715. DOI:10. 1021/ie060056n
[19]ZHAO Huazhang,SUN Yan,XU Lina,et al. Removal of Acid Orange 7 in simulated wastewater using a three-dimensional electrode reactor:Removal mechanisms and dye degradation pathway[J]. Chemosphere,2010,78(1):46. DOI:10. 1016/j.chemosphere. 2009. 10. 034
[20]LUO Haijian,LI Chaolin,SUN Xue,et al. Cathodic indirect oxidation of organic pollutant paired to anodic persulfate production[J]. Journal of Electroanalytical Chemistry,2017,792:110
[21]SONG Haoran,YAN Linxia,MA Jun,et al. Nonradical oxidation from electrochemical activation of peroxydisulfate at Ti/Pt anode:Efficiency,mechanism and influencing factors[J]. Water Res,2017,116:182. DOI:10. 1016/j. watres. 2017. 03. 035
[22]HORI H,YAMAMOTO A,HAYAKAWA E,et al. Efficient decomposition of environmentally persistent perfluorocarboxylic acids by use of persulfate as a photochemical oxidant[J]. Environmental Science&Technology,2005,39(7):2383
[23]LIU Jialu,ZHONG Shuang,SONG Yunpeng,et al. Degradation of tetracycline hydrochloride by electro-activated persulfate oxidation[J]. Journal of Electroanalytical Chemistry,2018,809:74
[24]SONGLIN W,NING Z. Removal of carbamazepine from aqueous solution using sono-activated persulfate process[J]. Ultrasonics Sonochemistry,2016,29:156. DOI:10. 1016/j. ultsonch. 2015.09. 008
[25]KOLTHOFF I M,MILLER I K. The chemistry of persulfate. 1. The kinetics and mechanism of the decomposition of the persulfate ions in aqueous medium[J]. Journal of the American Chemical Society,1951,73(7):3055. DOI:10. 1021/ja01151a024
[26]朱思瑞,高乃云,鲁仙,等.热激活过硫酸盐氧化降解水中双酚A[J].中国环境科学,2017,37(1):188ZHU Sirui,GAO Naiyun,LU Xian,et al. Degradation of bisphenol A in aqueous solution by thermally activated sulfate oxidation[J].China Environmental Science,2017,37(1):188. DOI:10. 3969/j. issn. 1000-6923. 2017. 01. 024
[27]史宸菲,薛瑞杰,李雨濛,等.不同活性炭活化过硫酸盐的效能及机理的规律研究[J].环境科学学报,2018,38(4):1501SHI Chenfei, XUE Ruijie, LI Yumeng, et al. Efficiency and mechanism of persulfate activation using different activated carbons[J]. Acta Scientiae Circumstantiae,2018,38(4):1501. DOI:10. 13671/j. hjkxxb. 2017. 0494
[28]冯玥,石文静,谭德俊,等.活性炭催化臭氧氧化处理染料废水生化出水研究[J].环境科学学报,2013,33(10):2724FENG Yue,SHI Wenjing,TAN Dejun,et al. Tertiary purification of biologically-treated effluent of dye-making wastewater by activated carbon catalytic ozonation[J]. Acta Scientiae Circunstantae,2013,33(10):2724. DOI:10. 13671/j. hjkxxb. 2013. 10. 019
[29]MORENO-CASTILLA C,FONTECHA-CAMARA M A,ALVAREZMERINO M A,et al. Activated carbon cloth as adsorbent and oxidation catalyst for the removal of amitrole from aqueous solution[J]. Adsorpation-Journal of the International Adsorption Society,2011,17(3):413
[30]ANIA C O,BEGUIN F. Electrochemical regeneration of activated carbon cloth exhausted with bentazone[J]. Environmental Science&Technology,2008,42(12):4500
[31]LIU Zhen, ZHAO Chun, WANG Pu, et al. Removal of carbamazepine in water by electro-activated carbon fiberperoxydisulfate:Comparison, optimization, recycle, and mechanism study[J]. Chemical Engineering Journal,2018,343:28
[32]BUXTON GEORGE V,GREENSTOCK CLIVE L,HELMAN W P,et al. Critical review of rate constants for reactions of hydrated electrons,hydrogen atoms and hydroxyl radicals(·OH/·O-)in aqueous solution[J]. Journal of Physical&Chemical Reference Data,1988,17(2):513
[33]NETA P,HUIE R E,ROSS A B. Rate constants for reactions of inorganic radicals in aqueous-solution[J]. Journal of Physics and Chemical Refference Data,1988,17(3):1027
[2]SCHEYTT T,MERSMANN P,LINDSTADT R,et al. Determination of sorption coefficients of pharmaceutically active substances carbamazepine,diclofenac,and ibuprofen,in sandy sediments[J].Chemosphere,2005,60(2):245
[3] ZHANG Yuqing, GEISSEN S, GAL C. Carbamazepine and diclofenac:Removal in wastewater treatment plants and occurrence in water bodies[J]. Chemosphere,2008,73(8):1151
[4]TERNES T A. Occurrence of drugs in German sewage treatment plants and rivers[J]. Water Research,1998,32(11):3245
[5]PAXEUS N. Removal of selected non-steroidal anti-inflammatory drugs(NSAIDs), gemfibrozil, carbamazepine, beta-blockers,trimethoprim and triclosan in conventional wastewater treatment plants in five EU countries and their discharge to the aquatic environment[J]. Water Science&Technology A Journal of the International Association on Water Pollution Research,2004,50(5):253. DOI:10. 2166/wst. 2004. 0335
[6]陈晓旸,薛智勇,吴丹,等.基于硫酸自由基的高级氧化技术及其在水处理中的应用[J].水处理技术,2009,35(5):16CHEN Xiaoyang, XUE Zhiyong, WU Dan, et al. Advanced oxidation technology based on sulfuric acid free radicals and its application in water treatment[J]. Technology Water Treatment,2009,35(5):16. DOI:10. 16796/j. cnki. 1000-3770. 2009. 05.005
[7]MATTA R,TLILI S,CHIRON S,et al. Removal of carbamazepine from urban wastewater by sulfate radical oxidation[J].Environmental Chemistry Letters,2011,9(3):347
[8]OLMEZ-HANCI T,ARSLAN-ALATON I. Comparison of sulfate and hydroxyl radical based advanced oxidation of phenol[J]. Chemical Engineering Journal,2013,224(1):10
[9]马京帅,吕文英,刘国光,等.吉非罗齐在热活化过硫酸盐体系中的降解机制研究[J].环境科学学报,2016,36(10):3774MA Jingshuai,LV Wenying,LIU Guoguang,et al. Degradation mechanism of gemfibrozil in heat-activated persulfate oxidation process[J]. Acta Scientiae Circumstantiae,2016,36(10):3774.DOI:10. 13671/j. hjkxxb. 2016. 0064
[10]SHU Hungyee,CHANG Mingchin,HUANG Shiwei. UV irradiation catalyzed persulfate advanced oxidation process for decolorization of Acid Blue 113 wastewater[J]. Desalination and Water Treatment,2015,54(4/5):1013
[11]高金龙,马玉琳,孟庆来,等.二价铁活化过硫酸盐降解土壤中十溴联苯醚[J].环境工程学报,2016(12):7339GAO Jinlong,MA Yulin,MENG Qinglai,et al. Degradation of decabromodiphenyl ether in soil by sulfate activated with ferrous ions[J]. Chinese Journal of Environmental Engineering,2016(12):7339. DOI:10. 12030/j. cjee. 201507210
[12]TEEL A L,AHMAD M,WATTS R J. Persulfate activation by naturally occurring trace minerals[J]. Journal of Hazardous Materials,2011,196(1):153
[13]QI Chengdu,LIU Xitao,LIN Chunye,et al. Degradation of sulfamethoxazole by microwave-activated persulfate:Kinetics,mechanism and acute toxicity[J]. Chemical Engineering Journal,2014,249:6
[14]SAPUTRA E,MUHAMMAD S,SUN H,et al. Activated carbons as green and effective catalysts for generation of reactive radicals in degradation of aqueous phenol[J]. RSC Advances,2013,3(44):21905
[15]施周,毕晨,周石庆,等.铁电极活化过硫酸盐对金橙G的降解[J].环境工程学报,2017,11(3):1335SHI Zhou,BI Chen,ZHOU Shiqing,et al. Degradation of iron electrode as sodium persulfate activator for orange G[J]. Chinese Journal of Environmental Engineering,2017,11(3):1335. DOI:10. 12030/j. cjee. 201511172
[16]YANG Shiying,YANG Xin,SHAO Xueting,et al. Activated carbon catalyzed persulfate oxidation of Azo dye acid orange 7 at ambient temperature[J]. Journal of Hazardous Materials,2011,186(1):659
[17]SANCHEZ-POLO M,VON G U,RIVERA-UTRILLA J. Efficiency of activated carbon to transform ozone into*OH radicals:Influence of operational parameters[J]. Water Research,2005,39(14):3189
[18]FARIA P C C,ORFAO J J M,PEREIRA M F R. Ozone decomposition in water catalyzed by activated carbon:Influence of chemical and textural properties[J]. Industrial&Engineering Chemistry Research, 2006, 45(8):2715. DOI:10. 1021/ie060056n
[19]ZHAO Huazhang,SUN Yan,XU Lina,et al. Removal of Acid Orange 7 in simulated wastewater using a three-dimensional electrode reactor:Removal mechanisms and dye degradation pathway[J]. Chemosphere,2010,78(1):46. DOI:10. 1016/j.chemosphere. 2009. 10. 034
[20]LUO Haijian,LI Chaolin,SUN Xue,et al. Cathodic indirect oxidation of organic pollutant paired to anodic persulfate production[J]. Journal of Electroanalytical Chemistry,2017,792:110
[21]SONG Haoran,YAN Linxia,MA Jun,et al. Nonradical oxidation from electrochemical activation of peroxydisulfate at Ti/Pt anode:Efficiency,mechanism and influencing factors[J]. Water Res,2017,116:182. DOI:10. 1016/j. watres. 2017. 03. 035
[22]HORI H,YAMAMOTO A,HAYAKAWA E,et al. Efficient decomposition of environmentally persistent perfluorocarboxylic acids by use of persulfate as a photochemical oxidant[J]. Environmental Science&Technology,2005,39(7):2383
[23]LIU Jialu,ZHONG Shuang,SONG Yunpeng,et al. Degradation of tetracycline hydrochloride by electro-activated persulfate oxidation[J]. Journal of Electroanalytical Chemistry,2018,809:74
[24]SONGLIN W,NING Z. Removal of carbamazepine from aqueous solution using sono-activated persulfate process[J]. Ultrasonics Sonochemistry,2016,29:156. DOI:10. 1016/j. ultsonch. 2015.09. 008
[25]KOLTHOFF I M,MILLER I K. The chemistry of persulfate. 1. The kinetics and mechanism of the decomposition of the persulfate ions in aqueous medium[J]. Journal of the American Chemical Society,1951,73(7):3055. DOI:10. 1021/ja01151a024
[26]朱思瑞,高乃云,鲁仙,等.热激活过硫酸盐氧化降解水中双酚A[J].中国环境科学,2017,37(1):188ZHU Sirui,GAO Naiyun,LU Xian,et al. Degradation of bisphenol A in aqueous solution by thermally activated sulfate oxidation[J].China Environmental Science,2017,37(1):188. DOI:10. 3969/j. issn. 1000-6923. 2017. 01. 024
[27]史宸菲,薛瑞杰,李雨濛,等.不同活性炭活化过硫酸盐的效能及机理的规律研究[J].环境科学学报,2018,38(4):1501SHI Chenfei, XUE Ruijie, LI Yumeng, et al. Efficiency and mechanism of persulfate activation using different activated carbons[J]. Acta Scientiae Circumstantiae,2018,38(4):1501. DOI:10. 13671/j. hjkxxb. 2017. 0494
[28]冯玥,石文静,谭德俊,等.活性炭催化臭氧氧化处理染料废水生化出水研究[J].环境科学学报,2013,33(10):2724FENG Yue,SHI Wenjing,TAN Dejun,et al. Tertiary purification of biologically-treated effluent of dye-making wastewater by activated carbon catalytic ozonation[J]. Acta Scientiae Circunstantae,2013,33(10):2724. DOI:10. 13671/j. hjkxxb. 2013. 10. 019
[29]MORENO-CASTILLA C,FONTECHA-CAMARA M A,ALVAREZMERINO M A,et al. Activated carbon cloth as adsorbent and oxidation catalyst for the removal of amitrole from aqueous solution[J]. Adsorpation-Journal of the International Adsorption Society,2011,17(3):413
[30]ANIA C O,BEGUIN F. Electrochemical regeneration of activated carbon cloth exhausted with bentazone[J]. Environmental Science&Technology,2008,42(12):4500
[31]LIU Zhen, ZHAO Chun, WANG Pu, et al. Removal of carbamazepine in water by electro-activated carbon fiberperoxydisulfate:Comparison, optimization, recycle, and mechanism study[J]. Chemical Engineering Journal,2018,343:28
[32]BUXTON GEORGE V,GREENSTOCK CLIVE L,HELMAN W P,et al. Critical review of rate constants for reactions of hydrated electrons,hydrogen atoms and hydroxyl radicals(·OH/·O-)in aqueous solution[J]. Journal of Physical&Chemical Reference Data,1988,17(2):513
[33]NETA P,HUIE R E,ROSS A B. Rate constants for reactions of inorganic radicals in aqueous-solution[J]. Journal of Physics and Chemical Refference Data,1988,17(3):1027