3DBER-S-Fe同步脱氮除磷及去除邻苯二甲酸酯的工艺特性
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摘要
为探究三维电极生物膜耦合硫铁新工艺(3DBER-S-Fe)脱氮除磷并同步去除邻苯二甲酸酯(PAEs)的工艺特性,在水力停留时间(HRT)分别为8、6、4 h条件下,研究分析了系统内总氮(TN)、总磷(TP)、邻苯二甲酸二丁酯(DBP)、邻苯二甲酸二(2-乙基)己酯(DEHP)、NO-3-N、SO2-4及pH的变化情况.结果表明,3DBER-S-Fe系统具有较好的脱氮除磷及PAEs去除效果.当水力停留时间为8、6、4 h时,TN去除率分别为80.99%、78.85%、64.76%;TP去除率分别为65.18%、67.17%、43.44%;DBP去除率分别为96.72%、97.32%、96.53%;DEHP去除率分别为91.89%、81.57%、74.30%.在3DBER-S-Fe系统内,存在异养、氢自养、硫自养反硝化脱氮过程,当HRT由8h缩短到4h时,单质硫可以弥补进水NO-3-N负荷增加所导致的反硝化电子供体相对不足问题,维持系统高效的脱氮效率;系统中海绵铁填料腐蚀产生的铁离子能够高效持续沉淀除磷;3DBER-S-Fe工艺结合了物理吸附、生物降解及电化学作用,使其在不同HRT条件下具有较高的DBP与DEHP去除率.
In order to explore the technological characteristics of the simultaneous removal of phthalate esters( PAEs) as well as nitrogen and phosphorus by the novel technology of three-dimensional biofilm-electrode coupled with iron / sulfur reactor( 3DBER-SFe),the changes of the total nitrogen( TN),total phosphorus( TP),DBP,DEHP,NO-3-N,SO2-4and pH value were analyzed under the hydraulic retention time( HRT) of 8 h,6 h and 4 h respectively. The results showed that 3DBER-S-Fe could remove nitrogen,phosphorus and PAEs effectively. Under the HRT of 8 h,6 h and 4 h,the removal rates of TN were 80. 99%,78. 85% and 64. 76%;TP were 65. 18%,67. 17% and 43. 44%; DBP were 96. 72%,97. 32% and 96. 53%; DEHP were 91. 89%,81. 57% and74. 30%, respectively. There were heterotrophic denitrification, hydrogen autotrophic denitrification and sulfur autotrophic denitrification processes in the 3DBER-S-Fe,the elemental sulfur could compensate for the relative shortage of denitrification electron donor caused by the increase of NO-3-N load in the influent as a result of maintaining a high efficiency of the denitrification system when the HRT was shortened from 8h to 4h; the iron ions produced by the corrosion of the sponge iron filler in the system had a sustainable and efficient function of removing phosphorus by precipitation; the 3DBER-S-Fe process combined the interactions of physical adsorption,biological degradation and electrochemical processes which supported its high removal rates of DBP and DEHP under the different HRT conditions.
In order to explore the technological characteristics of the simultaneous removal of phthalate esters( PAEs) as well as nitrogen and phosphorus by the novel technology of three-dimensional biofilm-electrode coupled with iron / sulfur reactor( 3DBER-SFe),the changes of the total nitrogen( TN),total phosphorus( TP),DBP,DEHP,NO-3-N,SO2-4and pH value were analyzed under the hydraulic retention time( HRT) of 8 h,6 h and 4 h respectively. The results showed that 3DBER-S-Fe could remove nitrogen,phosphorus and PAEs effectively. Under the HRT of 8 h,6 h and 4 h,the removal rates of TN were 80. 99%,78. 85% and 64. 76%;TP were 65. 18%,67. 17% and 43. 44%; DBP were 96. 72%,97. 32% and 96. 53%; DEHP were 91. 89%,81. 57% and74. 30%, respectively. There were heterotrophic denitrification, hydrogen autotrophic denitrification and sulfur autotrophic denitrification processes in the 3DBER-S-Fe,the elemental sulfur could compensate for the relative shortage of denitrification electron donor caused by the increase of NO-3-N load in the influent as a result of maintaining a high efficiency of the denitrification system when the HRT was shortened from 8h to 4h; the iron ions produced by the corrosion of the sponge iron filler in the system had a sustainable and efficient function of removing phosphorus by precipitation; the 3DBER-S-Fe process combined the interactions of physical adsorption,biological degradation and electrochemical processes which supported its high removal rates of DBP and DEHP under the different HRT conditions.
引文
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[19]Batchelor B,Lawrence A W.Autotrophic denitrification using elemental sulfur[J].Journal(Water Pollution Control Federation),1978,50(8):1986-2001.
[20]Bisogni Jr J J,Lawrence A W.Determination of submicrogram quantities of monomethyl mercury in aquatic samples[J].Environmental Science&Technology,1974,8(9):850-852.
[21]Bisogni Jr J J,Lawrence A W.Kinetics of mercury methylation in aerobic and anaerobic aquatic environments[J].Journal(Water Pollution Control Federation),1975,47(1):135-152.
[22]邱立平,马军,张立昕.水力停留时间对曝气生物滤池处理效能及运行特性的影响[J].环境污染与防治,2004,26(6):433-436.Qiu L P,Ma J,Zhang L X.Effect of hydraulic retention time on the treatment efficiency and operational characteristics of biological aerated filter[J].Environmental Pollution&Control,2004,26(6):433-436.
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[24]徐忠强,郝瑞霞,徐鹏程,等.硫铁填料和微电流强化再生水脱氮除磷的研究[J].中国环境科学,2016,36(2):406-413.Xu Z Q,Hao R X,Xu P C,et al.Research on enhanced denitrification and phosphorus removal from reclaimed water by useing sponge iron/sulfur composite fillers and low electrical current[J].China Environmental Science,2016,36(2):406-413.
[25]徐焕成,王平,赵雨,等.铝碳微电解法降解水中邻苯二甲酸酯[J].化工环保,2014,34(6):511-514.Xu H C,Wang P,Zhao Y,et al.Degradation of phthalate esters in water by Al-C microelectrolysis[J].Environmental Protection of Chemical Industry,2014,34(6):511-514.
[26]李升莲.人工湿地去除废水中有机微污染物邻苯二甲酸酯的研究[D].重庆:西南大学,2008.Li S L.Study on removal of organic micropollutants phthalic acid esters in constructed wetland treating sewage wastewater[D].Chongqing:Southwest University,2008.
[27]Huang J Y,Nkrumah P N,Li Y,et al.Chemical behavior of phthalates under abiotic conditions in landfills[M].In:Whitacre D M(ed.).Reviews of Environmental Contamination and Toxicology.New York:Springer,2013,224:39-52.
[28]Staples C A,Peterson D R,Parkerton T F,et al.The environmental fate of phthalate esters:a literature review[J].Chemosphere,1997,35(4):667-749.
[29]焦双吉.慢滤池去除污水中邻苯二甲酸二(2-乙基己基)酯的研究[D].北京:北京工业大学,2012.Jiao S J.Study on the removal of DI(2-Ethylhexyl)phthalate from sewage by A slow sand filter[D].Beijing:Beijing University of Technology,2012.
[30]Wu D L,Zheng P,Mahmood Q,et al.Isolation and characteristics of Arthrobacter sp.strain CW-1 for biodegradation of PAEs[J].Journal of Zhejiang University-Science A,2007,8(9):1469-1474.
[2]Schaum C,Lensch D,Cornel P.Water reuse and reclamation:a contribution to energy efficiency in the water cycle[J].Journal of Water Reuse and Desalination,2015,5(2):83-94.
[3]张杰,曹开朗.城市污水深度处理与水资源可持续利用[J].中国给水排水,2001,17(3):20-21.Zhang J,Cao K L.Advanced treatment of urban sewage and sustainable utilization of water resources[J].China Water&Wastewater,2001,17(3):20-21.
[4]董良飞,郗晓敏,余海静,等.MBR组合工艺脱氮除磷研究进展[J].中国给水排水,2010,26(4):24-28.Dong L F,Xi X M,Yu H J,et al.Research progress in nitrogen and phosphorus removal with MBR combined process[J].China Water&Wastewater,2010,26(4):24-28.
[5]池勇志,崔维花,苑宏英,等.不同源水和回用途径的再生水处理工艺的选择[J].中国给水排水,2012,28(18):22-26.Chi Y Z,Cui W H,Yuan H Y,et al.Selection of reclaimed water treatment processes under different source water qualities and reuse approaches[J].China Water&Wastewater,2012,28(18):22-26.
[6]张庆康,郝瑞霞,刘峰,等.不同再生水处理工艺出水水质回用途径适应性分析[J].环境工程学报,2013,7(1):91-96.Zhang Q K,Hao R X,Liu F,et al.Analysis about reuse approach adaptability for effluent quality from different reclaimed water treatment processes[J].Chinese Journal of Environmental Engineering,2013,7(1):91-96.
[7]郝瑞霞,张庆康,赵继成,等.固相萃取-气相色谱-质谱测定再生水中邻苯二甲酸酯类物质[J].环境污染与防治,2012,34(5):1-5,23.Hao R X,Zhang Q K,Zhao J C,et al.Determination of phthalates in reclaimed water by SPE-GC-MS[J].Environmental Pollution and Control,2012,34(5):1-5,23.
[8]徐鹏程,郝瑞霞,张娅,等.3BER-S工艺用于再生水深度脱氮同步去除PAEs的可行性[J].环境科学,2016,37(2):662-667.Xu P C,Hao R X,Zhang Y,et al.Feasibility of 3BER-S process for the deep denitrification in synch with the removal of PAEs from reclaimed water[J].Environmental Science,2016,37(2):662-667.
[9]王军良,徐超,庄晓伟,等.水中邻苯二甲酸酯污染现状及高级氧化降解技术研究[J].工业水处理,2011,31(4):5-10.Wang J L,Xu C,Zhuang X W,et al.Research on the present pollution situation and advanced oxidation degradation of phthalate esters in water[J].Industrial Water Treatment,2011,31(4):5-10.
[10]管策,郁达伟,郑祥,等.我国人工湿地在城市污水处理厂尾水脱氮除磷中的研究与应用进展[J].农业环境科学学报,2012,31(12):2309-2320.Guan C,Yu D W,Zheng X,et al.Removing nitrogen and phosphoros of effluent from wastewater treatment plants by constructed wetlands in china:an overview[J].Journal of AgroEnvironment Science,2012,31(12):2309-2320.
[11]肖文涛.污水生物脱氮除磷工艺的现状与发展[J].环境保护与循环经济,2010,30(11):59-62.Xiao W T.Status and development of biological nitrogen and phosphorus removal process for wastewater[J].Environmental Protection and Circular Economy,2010,30(11):59-62.
[12]郝瑞霞,张庆康,刘峰,等.再生水厂处理工艺对邻苯二甲酸酯去除效果分析[J].给水排水,2011,37(S1):74-78.Hao R X,Zhang Q K,Liu F,et al.Analysis of removal effects on phthalates in reclaimed water plants[J].Water&Wastewater Engineering,2011,37(S1):74-78.
[13]李素梅,郝瑞霞,孟成成.三维电极生物膜反应器低温启动试验研究[J].中国给水排水,2013,29(5):101-105.Li S M,Hao R X,Meng C C.Start-up of three-dimensional electrode biofilm reactor at low temperature[J].China Water&Wastewater,2013,29(5):101-105.
[14]郝瑞霞,王建超,孟成成,等.电流对三维电极生物膜耦合硫自养脱氮工艺的影响[J].北京工业大学学报,2015,41(6):919-925.Han R X,Wang J C,Meng C C,et al.Influence of electric current on coupling)3-dimensional biofilm-electrode with sulfur autotrophic denitrification[J].Journal of Beijing University of Technology,2015,41(6):919-925.
[15]王建超,郝瑞霞,孟成成,等.3DBER-S反硝化脱氮性能及其菌群特征[J].环境科学研究,2015,28(2):310-317.Wang J C,Hao R X,Meng C C,et al.Study on performance and bacterial community of coupling 3-dimensional biofilmelectrode with sulfur autotrophic denitrification[J].Research of Environmental Sciences,2015,28(2):310-317.
[16]常玉梅,杨琦,郝春博,等.城市污水厂活性污泥强化自养反硝化菌研究[J].环境科学,2011,32(4):1210-1216.Chang Y M,Yang Q,Hao C B,et al.Experimental study of autotrophic denitrification bacteria through bioaugmentation of activated sludge from municipal wastewater plant[J].Environmental Science,2011,32(4):1210-1216.
[17]胡传侠,杨昌柱,杨群,等.固定化三维电极-生物膜法去除污水中硝酸盐氮[J].环境科学与技术,2008,31(2):83-87.Hu C X,Yang C Z,Yang Q,et al.Study on removal of nitrate from by secondary effluent immobilized three-dimension electrodebiofilm reactor[J].Environmental Science&Technology,2008,31(2):83-87.
[18]王海燕,蔡海军.COD与TOC相关性理论研究[J].河南城建学院学报,2011,20(2):36-40.Wang H Y,Cai H J.Relevant research of TOC and COD in organic wastewater[J].Journal of Henan University of Urban Construction,2011,20(2):36-40.
[19]Batchelor B,Lawrence A W.Autotrophic denitrification using elemental sulfur[J].Journal(Water Pollution Control Federation),1978,50(8):1986-2001.
[20]Bisogni Jr J J,Lawrence A W.Determination of submicrogram quantities of monomethyl mercury in aquatic samples[J].Environmental Science&Technology,1974,8(9):850-852.
[21]Bisogni Jr J J,Lawrence A W.Kinetics of mercury methylation in aerobic and anaerobic aquatic environments[J].Journal(Water Pollution Control Federation),1975,47(1):135-152.
[22]邱立平,马军,张立昕.水力停留时间对曝气生物滤池处理效能及运行特性的影响[J].环境污染与防治,2004,26(6):433-436.Qiu L P,Ma J,Zhang L X.Effect of hydraulic retention time on the treatment efficiency and operational characteristics of biological aerated filter[J].Environmental Pollution&Control,2004,26(6):433-436.
[23]陈丹,王弘宇,宋敏,等.生物陶粒反应器的氢自养反硝化研究[J].环境科学,2013,34(10):3986-3991.Chen D,Wang H Y,Song M,et al.Study on hydrogen autotrophic denitrification of bio-ceramic reactor[J].Environmental Science,2013,34(10):3986-3991.
[24]徐忠强,郝瑞霞,徐鹏程,等.硫铁填料和微电流强化再生水脱氮除磷的研究[J].中国环境科学,2016,36(2):406-413.Xu Z Q,Hao R X,Xu P C,et al.Research on enhanced denitrification and phosphorus removal from reclaimed water by useing sponge iron/sulfur composite fillers and low electrical current[J].China Environmental Science,2016,36(2):406-413.
[25]徐焕成,王平,赵雨,等.铝碳微电解法降解水中邻苯二甲酸酯[J].化工环保,2014,34(6):511-514.Xu H C,Wang P,Zhao Y,et al.Degradation of phthalate esters in water by Al-C microelectrolysis[J].Environmental Protection of Chemical Industry,2014,34(6):511-514.
[26]李升莲.人工湿地去除废水中有机微污染物邻苯二甲酸酯的研究[D].重庆:西南大学,2008.Li S L.Study on removal of organic micropollutants phthalic acid esters in constructed wetland treating sewage wastewater[D].Chongqing:Southwest University,2008.
[27]Huang J Y,Nkrumah P N,Li Y,et al.Chemical behavior of phthalates under abiotic conditions in landfills[M].In:Whitacre D M(ed.).Reviews of Environmental Contamination and Toxicology.New York:Springer,2013,224:39-52.
[28]Staples C A,Peterson D R,Parkerton T F,et al.The environmental fate of phthalate esters:a literature review[J].Chemosphere,1997,35(4):667-749.
[29]焦双吉.慢滤池去除污水中邻苯二甲酸二(2-乙基己基)酯的研究[D].北京:北京工业大学,2012.Jiao S J.Study on the removal of DI(2-Ethylhexyl)phthalate from sewage by A slow sand filter[D].Beijing:Beijing University of Technology,2012.
[30]Wu D L,Zheng P,Mahmood Q,et al.Isolation and characteristics of Arthrobacter sp.strain CW-1 for biodegradation of PAEs[J].Journal of Zhejiang University-Science A,2007,8(9):1469-1474.