臭氧、活性炭、超滤及联用工艺去除邻苯二甲酸酯的效能与机理
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摘要
为提高水厂对邻苯二甲酸酯类环境激素的处理效果,研究臭氧、活性炭、超滤及2种联用工艺对PAEs(DMP、DEP、DBP、DEHP)的去除效果及降解机理.结果表明,单独的臭氧氧化、活性炭吸附、超滤过滤均能去除部分PAEs,最优工艺参数:臭氧投加量8 mg·L-1,空床停留时间15 min,超滤操作压力0.01 MPa.当PAEs进水浓度分别为10μg·L-1、15μg·L-1、20μg·L-1、25μg·L-1时,臭氧—活性炭工艺的PAEs综合去除率为55.19%~66.12%,小分子的DMP、DEP检出浓度均低于3μg·L-1,处理效果优于大分子量的DBP、DEHP.活性炭—超滤工艺对大分子PAEs的吸附截留作用明显,各PAEs物质的检出浓度介于0~3.11μg·L-1.对比2种联用工艺可知,在低中高3种PAEs进水浓度下,活性炭—超滤工艺的PAEs综合去除率及末端PAEs出水浓度均优于臭氧—活性炭工艺的处理效果,超滤作为第三代净水工艺有着良好的技术优势.
In order to improve the performance of environmental hormone in the treatment of phthalic acid esters( PAEs),the removal efficiency and degradation mechanism of PAEs( DMP,DEP,DBP,DEHP) by ozone,activated carbon,ultrafiltration and two kinds of combined processes were studied in this paper. The results showed that the single ozone oxidation,activated carbon adsorption,ultrafiltration filtration can remove part of PAEs,the Optimum ultrafiltration operation pressure 0. 01 MPa. When the influent concentration of PAEs is10,15,20,25 μg · L-1,the comprehensive removal rate of PAEs from ozone activated carbon process is55. 19% ~ 66. 12%,the detection concentration of small molecules DMP and DEP is lower than 3 μg·L-1,and the treatment effect is better than that of DBP,DEHP. Activated carbon ultrafiltration process has a significant effect on the filtration of high molecular weight PAEs,and the detection concentration of PAEs is 0 ~ 3. 11μg·L-1. By a comparison on two kinds of combination process,in low,high influent PAEs concentration,activated carbon—ultrafiltration process on the PAEs removal rate and PAEs end of the effluent concentration are better than that of ozone—activated carbon process treatment. Ultrafiltration,as the third generation water purification process,has a good technological advantage.
In order to improve the performance of environmental hormone in the treatment of phthalic acid esters( PAEs),the removal efficiency and degradation mechanism of PAEs( DMP,DEP,DBP,DEHP) by ozone,activated carbon,ultrafiltration and two kinds of combined processes were studied in this paper. The results showed that the single ozone oxidation,activated carbon adsorption,ultrafiltration filtration can remove part of PAEs,the Optimum ultrafiltration operation pressure 0. 01 MPa. When the influent concentration of PAEs is10,15,20,25 μg · L-1,the comprehensive removal rate of PAEs from ozone activated carbon process is55. 19% ~ 66. 12%,the detection concentration of small molecules DMP and DEP is lower than 3 μg·L-1,and the treatment effect is better than that of DBP,DEHP. Activated carbon ultrafiltration process has a significant effect on the filtration of high molecular weight PAEs,and the detection concentration of PAEs is 0 ~ 3. 11μg·L-1. By a comparison on two kinds of combination process,in low,high influent PAEs concentration,activated carbon—ultrafiltration process on the PAEs removal rate and PAEs end of the effluent concentration are better than that of ozone—activated carbon process treatment. Ultrafiltration,as the third generation water purification process,has a good technological advantage.
引文
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[19]何嘉莉,张晓娜,陈丽珠,等.生物活性炭与臭氧/活性炭工艺控制DBPs前体物比较[J].中国给水排水,2016,32(9):50-52.HE J L,ZHANG X N,CHEN L Z,et al.Comparative analysis on control of disinfection by-products precursors by biological activated carbon process and ozone/activated carbon process[J].Chin Water Wastwater,2016,32(9):50-52.
[20]鲁金凤,杜智,张爱平,等.高级氧化组合工艺协同净化微污染水的示范生产实验[J].哈尔滨工业大学学报,2017,49(2):20-25.LU J F,DU Z,ZHANG A P,et al.Demonstrative and productive experimental research on synergistic purificationof the micro-polluted water by advanced oxidation combined process[J].J Harbin Inst Tech,2017,49(2):20-25.
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[22]褚耀飞.电化学与臭氧联用技术降解水中DEP[D].上海:上海应用技术大学,2016.CHU Y F.Degradetion of diethyl phthalate by the technology of electrochemistry coupled with ozone[D].Shanghai:Shanghai Institute of Technology,2016.
[23]李怀茂.臭氧+活性炭/沸石组合工艺去除饮用水中邻苯二甲酸酯研究[D].重庆:重庆大学,2009.LI H M.Study on removal of phthalate esters from drinking water using combinatorial process of O3+GAC/Zeolite[D].Chongqing:Chongqing University,2009.
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[2]李彬,吴山,梁金明,等.珠江三角洲典型区域农产品中邻苯二甲酸酯(PAEs)污染分布特征[J].环境科学,2016,37(1):317-324.LI B,WU S,LIANG J M,et al.Distribution characteristics and risk assessment of Phthalic Acid Esters in agricultural products around the Pearl River Delta,south China[J].Environ Sci,2016,37(1):317-324.
[3]骆祝华,黄翔玲,叶德赞.环境内分泌干扰物——邻苯二甲酸酯的生物降解研究进展[J].应用与环境生物学报,2008,14(6):890-897.LUO Z H,HUANG X L,YE D Z.Advances in research of biodegradation of environmental endocrine disruptors:Phthalate esters[J].J Appl Environ Biol,2008,14(6):890-897.
[4]薛琦,朱光灿,戴小冬,等.臭氧—生物活性炭工艺对微污染长江原水中有机物的去除特性[J].净水技术,2015,34(4):36-41.XUE Q,ZHU G C,DAI X D,et al.Characteristics of organic matter removal of micro-polluted raw water from Yangtze river with Ozone-Biological Activated Carbon(O3-BAC)treatment processes[J].Water Pur Tech,2015,34(4):36-41.
[5]乔铁军.活性炭—超滤复合工艺去除水中典型PPCPs的效能与机理[D].北京:清华大学,2011.QIAO T J.Performance and mechanism of typical Pharmaceuticals and Personal Care Products removal from water by the hybrid processes of granular activated carbon and ultrafiltration[D].Beijing:Tsinghua University,2011.
[6]杨洁.臭氧—活性炭工艺中臭氧投加量优化试验研究[D].广州:华南理工大学,2012.YANG J.Study on ozone dosage optimal control in O3-BAC process[D].Guangzhou:South China University of Technology,2012.
[7]NI C H,CHEN J N,YANG P Y.Catalytic ozonation of 22 dichlorophenol bymetallic ions[J].Water Sci Tech,2003,47(1):77-82.
[8]KIMURA K,MAEDA T,YAMAMURA H,et al.Irreversible membrane fouling in microfiltration membranes filtering coagulated surface water[J].J Memb Sci,2008,320(1/2):356-362.
[9]张剑桥,马军,迟惠中,等.基于压力衰减的超滤膜急性与慢性物理破损评价[J].哈尔滨工业大学学报,2016,48(2):33-37.ZHANG J Q,MA J,CHI H Z,et al.Evaluation of sudden and slow physical damage of ultrafiltration membrane based on pressure declination monitoring[J].J Harbin Inst Tech,2016,48(2):33-37.
[10]PANDOLFO A G,AMINI-AMOLI M,KILLINGLEY J S.Activated carbons prepared from shells of different coconut varieties[J].Carbon,1994,32(5):1015-1019.
[11]刘宏英,陈秋丽,张朝升,等.固相萃取—高效液相色谱法同时测定水中三种邻苯二甲酸酯[J].中国给水排水,2016,32(8):122-126.LIU H Y,CHEN Q L,ZHANG C S,et al.Simultaneous determination of three phthalic acid esters in water by high performance liquid chromatography with solid phase extraction[J].Chin Water Wastw,2016,32(8):122-126.
[12]晏云鹏,全学军,程治良,等.垃圾焚烧发电厂渗滤液生化出水的催化臭氧氧化处理[J].环境工程学报,2015,9(1):219-224.YAN Y P,QUAN X J,CHENG Z L,et al.Catalytic ozonation of biologically treated leachate from municipal solid waste incineration power plan[J].J Environ Eng,2015,9(1):219-224.
[13]贺道红.臭氧—生物活性炭与微曝气—生物活性炭深度处理效果对比研究[D].上海:同济大学,2006.HE D H.Study on comprarison of adavanced treatment between Ozone-BAC and microaertion-BAC processes[D].Shanghai:Tongji University,2006.
[14]胡明城.粒状活性炭固定床吸附系统的重要设计参数——空床接触时间(EBCT)[J].化工给排水设计,1998(3):17-18.HU M C.The important design parameters of granular activated carbon fixed bed adsorption system of the empty bed contact time(EBCT)[J].Chem Water Suppl Drainag Desig,1998(3):17-18.
[15]黄韵清,孙傅,曾思育,等.污水深度处理中超滤工艺对有机物的截留模型[J].中国环境科学,2015,35(2):420-426.HUANG Y Q,SUN F,ZENG S Y,et al.Modeling organics rejection during ultrafiltration in advanced wastewater treatment[J].Chin Environ Sci,2015,35(2):420-426.
[16]ALVENTOSA D E,BARREDO D S,ALCAINA M M,et al.Ultrafiltration technology with a ceramic membrane for reactive dye removal:Optimization of membrane performance[J].J Hazard Mater,2012,209-210(1):492-500.
[17]莫颖慧.污水纳滤深度处理的膜污染及其对微量有机物截留的影响[D].北京:清华大学,2013.MO Y H.Fouling and its effect on rejection of micro-organic pollutants during nanofiltration for advanced treatment of wastewater[D].Beijing:Tsinghua University,2013.
[18]高旭,余仲勋,郭劲松,等.臭氧—生物活性炭工艺对饮用水中邻苯二甲酸酯类的去除中试研究[J].环境工程学报,2011,5(8):1773-1778.GAO X,YU Z X,GUO J S,et al.Pilot study on removal of phthalate esters from drinking water using ozone-zeolite/activated carbon filler technique[J].Chin J Environ Eng,2015,5(8):219-224.
[19]何嘉莉,张晓娜,陈丽珠,等.生物活性炭与臭氧/活性炭工艺控制DBPs前体物比较[J].中国给水排水,2016,32(9):50-52.HE J L,ZHANG X N,CHEN L Z,et al.Comparative analysis on control of disinfection by-products precursors by biological activated carbon process and ozone/activated carbon process[J].Chin Water Wastwater,2016,32(9):50-52.
[20]鲁金凤,杜智,张爱平,等.高级氧化组合工艺协同净化微污染水的示范生产实验[J].哈尔滨工业大学学报,2017,49(2):20-25.LU J F,DU Z,ZHANG A P,et al.Demonstrative and productive experimental research on synergistic purificationof the micro-polluted water by advanced oxidation combined process[J].J Harbin Inst Tech,2017,49(2):20-25.
[21]刘军,王珂,贾瑞宝,等.臭氧—活性炭工艺对饮用水中邻苯二甲酸酯的去除[J].环境科学,2003,24(4):77-80.LIU J,WANG K,JIA R B,et al.Removal of phthalate esters from drinking water using ozone-GAC process[J].Environ Sci,2003,24(4):77-80.
[22]褚耀飞.电化学与臭氧联用技术降解水中DEP[D].上海:上海应用技术大学,2016.CHU Y F.Degradetion of diethyl phthalate by the technology of electrochemistry coupled with ozone[D].Shanghai:Shanghai Institute of Technology,2016.
[23]李怀茂.臭氧+活性炭/沸石组合工艺去除饮用水中邻苯二甲酸酯研究[D].重庆:重庆大学,2009.LI H M.Study on removal of phthalate esters from drinking water using combinatorial process of O3+GAC/Zeolite[D].Chongqing:Chongqing University,2009.
[24]KIM I,TANAKA H.Use of ozone-based processes for the removal of pharmaceuticals detected in a wastewater treatment plant[J].Water Environ Res,2010,82(4):294-301.
[25]李昌贤,秦延武.煤质活性炭[M].北京:煤炭工业出版社,1993.LI C X,QIN Y W.Coaly activated carbon[M].Beijing:Press of Coal Industry,1993.
[26]李清雪,李曼,赵海萍,等.超滤去除二级出水中PAEs的试验研究[J].河北师范大学学报,2008,32(5):656-665.LI Q X,LI M,ZHAO H P,et al.Experimental study on ultrafiltration to remove PAEs in water level two[J].J Hebei Nor Univ,2008,32(5):656-665.
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