污水处理厂各构筑物中多溴联苯醚的去除

doi:10.3969/j.issn.1000-1565.2020.02.005

摘要/Abstract

摘要： 以保定污水处理厂为研究对象,分别采集了夏、冬两季污水处理厂内各个构筑物中的污水及生物反应池中的污泥样本,通过萃取、净化和浓缩后,利用GC和GC-MS检测出10种多溴联苯醚(PBDEs),通过对水、泥以及夏、冬两季各构筑物中PBDEs含量比较,探讨了PBDEs的分布、迁移转化规律及去除PBDEs的影响因素.结果表明:1)夏季污水中(进水-出水)PBDEs的质量浓度为43.2~315.8 ng/L,生物反应池中的污泥样品质量分数为2 361.1~3 186.0 ng/g;冬季污水中(进水-出水)PBDEs的质量浓度为108.1~403.5 ng/L,生物反应池中的污泥样品质量分数为2 247.8~2 782.7 ng/g.2)初沉池(夏季53.55%,冬季38.19%)和生物反应池(夏季51.13%,冬季36.61%)中PBDEs的去除效率最高;夏季(86.30%)比冬季(73.22%)污水中的PBDEs去除效率略高.3)构筑物中BDE-209是主导同类物,BDE-100和BDE-99则是仅次于BDE-209的另外2种主要同类物.该研究结果为监控和评估污水处理厂的PBDEs及其他持久性有机污染物的去除效率提供参考.

关键词: 多溴联苯醚, 污水处理厂, 迁移转化, 污泥

Abstract: Taking Baoding sewage-treatment plants research object,the sewage and biological sludge in the various buildings of the sewage-treatment plant were collected in the summer and winter.After the collected samples were extracted,purified and determined,10 congeners of PBDEs were detected in these samples by GC and GC-MS.Through comparison of PBDEs concentration in the sewage and sludge from two seasons(in summer and winter),the distribution,migration and transformation of PBDEs and factors influencing the removal of PBDEs were discussed.The results showed that: 1)The concentrations of PBDEs in sewage(inlet to outlet)ranged from 43.2 to 315.8 ng/L,and the concentrations of sludge in bioreactor were between 2 361.1 and 3 186.0 ng/g in summer;in contrast with summer,in winter the concentrations of PBDEs in sewage(inlet to outlet)and sludge ranged from 108.1 to 403.5 ng/L,and 2 247.8 to 2 782.7 ng/g,- DOI:10.3969/j.issn.1000-1565.2020.02.005污水处理厂各构筑物中多溴联苯醚的去除何增浩,王晓冰,刘芃岩,巩一潮,朱爱雪,牛玥(河北大学化学与环境科学学院,河北保定 071002)摘要:以保定污水处理厂为研究对象,分别采集了夏、冬两季污水处理厂内各个构筑物中的污水及生物反应池中的污泥样本,通过萃取、净化和浓缩后,利用GC和GC-MS检测出10种多溴联苯醚(PBDEs),通过对水、泥以及夏、冬两季各构筑物中PBDEs含量比较,探讨了PBDEs的分布、迁移转化规律及去除PBDEs的影响因素.结果表明:1)夏季污水中(进水-出水)PBDEs的质量浓度为43.2~315.8 ng/L,生物反应池中的污泥样品质量分数为2 361.1~3 186.0 ng/g;冬季污水中(进水-出水)PBDEs的质量浓度为108.1~403.5 ng/L,生物反应池中的污泥样品质量分数为2 247.8~2 782.7 ng/g.2)初沉池(夏季53.55%,冬季38.19%)和生物反应池(夏季51.13%,冬季36.61%)中PBDEs的去除效率最高;夏季(86.30%)比冬季(73.22%)污水中的PBDEs去除效率略高.3)构筑物中BDE-209是主导同类物,BDE-100和BDE-99则是仅次于BDE-209的另外2种主要同类物.该研究结果为监控和评估污水处理厂的PBDEs及其他持久性有机污染物的去除效率提供参考.关键词:多溴联苯醚;污水处理厂;迁移转化;污泥中图分类号:X832 文献标志码:A 文章编号:1000-1565(2020)02-0137-07Removal of polybrominated diphenyl ethers in various buildings of sewage treatment plantHE Zenghao,WANG Xiaobing,LIU Pengyan,GONG Yichao,ZHU Aixue,NIU Yue(College of Chemistry and Environmental Science,Hebei University,Baoding 071002,China)Abstract: Taking Baoding sewage-treatment plants research object,the sewage and biological sludge in the various buildings of the sewage-treatment plant were collected in the summer and winter.After the collected samples were extracted,purified and determined,10 congeners of PBDEs were detected in these samples by GC and GC-MS.Through comparison of PBDEs concentration in the sewage and sludge from two seasons(in summer and winter),the distribution,migration and transformation of PBDEs and factors influencing the removal of PBDEs were discussed.The results showed that: 1)The concentrations of PBDEs in sewage(inlet to outlet)ranged from 43.2 to 315.8 ng/L,and the concentrations of sludge in bioreactor were between 2 361.1 and 3 186.0 ng/g in summer;in contrast with summer,in winter the concentrations of PBDEs in sewage(inlet to outlet)and sludge ranged from 108.1 to 403.5 ng/L,and 2 247.8 to 2 782.7 ng/g,- 收稿日期:2019-07-21 基金项目:国家自然科学基金资助项目(21377033);河北省自然科学基金资助项目(B2018201224) 第一作者:何增浩(1995—),男,河北邢台人,河北大学在读硕士研究生,主要从事持久性有机污染物迁移转化研究.E-mail:949594564@qq.com 通信作者:刘芃岩(1964—),女,河北保定人,河北大学教授,主要从事环境中典型污染物的生成降解与迁移转化研究.E-mail:hbupyliu@163.com第2期何增浩等:污水处理厂各构筑物中多溴联苯醚的去除respectively.2)The removal efficiencies of PBDEs were higher in the primary sedimentation tank(summer: 53.55%,winter: 38.19%)and the bioreactor tank(summer: 51.13%,winter: 36.61%)than that of other buildings;The removal efficiency of PBDEs in sewage was slightly higher in summer(86.30%)than in winter(73.22%).3)BDE-209 was the dominant congener in the building followed by BDE-100 and BDE-99.The results of this study provide a reference for monitoring and evaluating the removal efficiency of PBDEs and other POPs in sewage-treatment plants.

Key words: polybrominated diphenyl ethers, sewage treatment plant, migration conversion, sludge

中图分类号:

X832

何增浩,王晓冰,刘芃岩,巩一潮,朱爱雪,牛玥. 污水处理厂各构筑物中多溴联苯醚的去除[J]. 河北大学学报(自然科学版), 2020, 40(2): 137-143.

HE Zenghao,WANG Xiaobing,LIU Pengyan,GONG Yichao,ZHU Aixue,NIU Yue. Removal of polybrominated diphenyl ethers in various buildings of sewage treatment plant[J]. Journal of Hebei University (Natural Science Edition), 2020, 40(2): 137-143.

参考文献

[1] 林海涛,李琦路,张千,等.中国8个城市大气多溴联苯醚的污染特征及人体暴露水平[J].环境科学,2016,37(1): 10-15.DOI:10.13227/j.hjkx.2016.01.002.
[2] STOKER T E,COOPER R L,LAMBRIGHT C S,et al.In vivo and in vitro ant-iandrogenic effects of DE-71,a commercial polybrominated diphenyl ether(PBDE)mixture[J].Toxicol Appl Pharmaco,2005,207: 78-88.DOI:10.1016/j.taap.2005.05.010.
[3] 刘早玲,张建清.多溴联苯醚对甲状腺激素干扰毒性的研究进展[J].环境与职业医学,2010,27(2): 107-112.DOI:10.13213/j.cnki.jeom.2010.02.013.
[4] 张慧慧,于国伟,牛静萍,等.多溴联苯醚健康效应的研究进展[J].环境与健康杂志,2011,28(12): 1124-1127.DOI:10.16241/j.cnki.1001-5914.2011.12.034.
[5] 杨华伟,胡伟,冯正,等.多溴二苯醚及其代谢物的内分泌干扰活性和构效关系研究进展[J].生态毒理学报,2009,4(2): 164-173.DOI:1673 - 5897(2009)2 - 164 - 10.
[6] HAMERS T,KAMSTRA J H,SONNEVELD E,et al.Biotransformation of brominated flame retardants into potentially endocrine-disrupting metabolites,with special attention to 2,2’,4,4’-tetrabromodiphenyl ether(BDE-47)[J].Molecular Nutrition & Food Research,2008,52: 284-298.
[7] LAU F K,CHARLES M J,CAHILL T M.Evaluation of gas-stripping methods for the determination of Henrys law constants for polybrominated diphenyl ethers and polychlorinated biphenyls[J].Journal of Chemical and Engineering Data,2006,51(3): 871-878.DOI:10.1016/j.jpba.2006.08.002.
[8] 金军,王英,刘伟志,等.莱州湾地区土壤及底泥中多溴联苯醚水平及其分布[J].环境科学学报,2008,28(7): 1463-1468.DOI:10.13671/j.hjkxxb.2008.07.028.
[9] 薛南冬,陈宣宇,刘寒冰.双金属系统还原脱溴降解多溴联苯醚(PBDEs)研究进展[J].环境工程学报,2016,10(05):2157-2167.DOI:10.12030/j.cjee.201412097.
[10] DE WIT C A.An overview of brominated flame retardants in the environment[J].Chemosphere,2002,46(5): 583-624.DOI:10.1016/S0045-6535(01)00225-9.
[11] 周鹏,于慧娟,赵建华,等.典型污水处理厂中多溴联苯醚的分布特征、迁移及负荷研究[J].环境科学学报,2016,36(4): 1248-1259.DOI:10.13671/j.hjkxxb.2015.0601.
[12] 孟祥周,杨超,潘兆宇,等.污水及污泥中多溴联苯醚的研究进展[J].环境科学与技术,2011,34(02):102-106.DOI:1003-6504(2011)02-0102-05.
[13] 孟得磊,马利民.A/O工艺处理生活污水中PBDEs分布特征[J].环境科学与技术,2011,34(07):10-11.DOI:1003-6504(2011)07-0010-02.
[14] JIANG J G,ZHAO H X,SUN S B,et al.Occurrence and profiles of halogenated phenols,polybrominated diphenyl ethers and hydroxylated polybrominated diphenyl ethers in the effluents of waste water treatment plants around Huang-Bo Sea,North China[J].Science of the Total Environment,2018,622-623:1-7.DOI:10.1016/j.scitotenv.2017.11.323.
[15] LI B,SUN S J,HUO C Y,et al.Occurrence and fate of PBDEs and novel brominated flame retardants in a wastewater treatment plant in Harbin,China [J].Environmental Science and Pollution Research,2016,23(19):19246-19256.DOI:10.1007/s11356-016-7142-y.
[16] RAN Y,YANG J,LIU Y J,et al.Levels,compositions,and inventory of polybrominated diphenyl ethers in sewage sludge of Guangdong Province,South China[J].Environmental science and pollution research international,2013,20(12):8780-8789.DOI:10.1007/s11356-013-1834-3.
[17] JUAN S,JORDI B,GEMMA V,et al.Determination and occurrence of phthalates,alkyl phenols,bisphenol A,PBDEs,PCBs and PAHs in an industrial sewage grid discharging to a Municipal Wastewater Treatment Plant[J].Science of the Total Environment,2009,407(13):4157-4167.DOI:10.1016/j.scitotenv.2009.03.016.
[18] DEMIRTEPE H,IMAMOGLU I.Levels of polybrominated diphenyl ethers and hexabromocyclododecane in treatment plant sludge: Implications on sludge management[J].Chemosphere,2019,221.DOI:10.1016/j.chemosphere.2019.01.060.
[19] BRADLEY O C,NICHOLA A P,ROBERT K S,et al.Investigating the distribution of polybrominated diphenyl ethers through an Australian wastewater treatment plant[J].Science of the Total Environment,2009,408(7)1604-1611.DOI:10.1016/j.scitotenv.2009.11.059.
[20] WANG Y W,JIANG G B,LAM P K S,et al.Polybrominated diphenyl ether in the East Asian environment: a critical review[J].Environment International,2007,33(7): 963-973.DOI:10.1016/j.envint.2007.11.001.
[21] NORTH K D.Tracking polybrominated diphenyl ether releases in a wastewater treatment plant effluent,Palo Alto,California[J].Environmental Science&Technology,2004,38(17): 4484-4488.DOI:10.1021/es049627y.
[22] RAYNE S,IKONOMOU M G.Polybrominated diphenyl ethers in an advanced wastewater treatment plant.Part 1: Concentrations,patterns,and influence of treatment processes[J].Journal of Environmental Engineering and Science,2005,4(5): 353-367.DOI:10.1016/j.scitotenv.2005.04.014.
[23] PENG X Z,TANG C M,YU Y Y,et al.Concentrations,transport,fate,and releases of polybrominated diphenyl ethers in sewage treatment plants in the Pearl River Delta,South China[J].Environment International,2008,35(2): 303-309.DOI:10.1016/j.envint.2008.07.021.
[24] YANG C,MENG X Z,CHEN L,et al.Polybrominated diphenyl ethers in sewage sludge from Shanghai,China: possible ecological risk applied to agricultural land[J]. Chemosphere,2011,85(3):418-423.DOI:10.1016/j.chemosphere.2011.07.068.