江苏省典型化工园区7种邻苯二甲酸酯污染特征及风险评估

doi:10.19741/j.issn.1673-4831.2023.0143

摘要/Abstract

摘要： 为评价江苏省典型化工园区邻苯二甲酸酯（PAEs）污染特征及风险等级，于2022年12月对江苏常州、苏州、泰州和南通4市5个化工园区饮用水、地表水、污水处理厂进出水、土壤和沉积物进行采样，利用气相色谱-质谱仪测定各环境介质样品中PAEs浓度。结果表明，5个化工园区不同环境介质中主要检出PAEs为邻苯二甲酸二（2-乙基己基）酯（DEHP）、邻苯二甲酸二丁酯（DBP）、邻苯二甲酸二异丁酯（DIBP）和邻苯二甲酸二辛酯（DNOP），水环境中总PAEs质量浓度范围为ND~13 757 ng·L^-1，平均质量浓度为1 369 ng·L^-1；沉积物中总PAEs范围为78.4~2 618 μg·kg^-1，平均为661 μg·kg^-1；土壤中总PAEs范围为56.7~1 329 μg·kg^-1，平均为442 μg·kg^-1。南通、泰州地表水和饮用水以及泰州污水处理厂排口等点位PAEs检出浓度均较高，同时这些区域土壤和沉积物点位PAEs检出浓度也较高。基于风险熵值法的PAEs风险评估结果表明，5个化工园地表水、土壤和沉积物中PAEs呈现中、高程度风险；PAEs在污水处理厂中总体呈现高风险。健康风险评价结果表明，5个化工园区饮用水及周边水源地水体中PAEs健康风险熵（Q_RH）为0~0.191 2，PAEs在南通饮用水中表现出中等健康风险，在其他地区表现为较低风险。总体来说，PAEs在南通、泰州的环境介质中污染程度最高，且具有中等以上环境风险，应引起足够重视，有必要进一步开展PAEs在这些区域的污染排放溯源，采取有效措施控制PAEs向环境过量排放。

关键词: 邻苯二甲酸酯, 化工园区, 污染特征, 风险评估

Abstract: This study aimed to evaluate the pollution characteristics and risks of phthalate esters (PAEs) in typical chemical industry parks in Jiangsu Province. Samples were collected of drinking water, surface water, raw water and effluent from sewage treatment plants, and soil and sediment from five chemical industry parks in Changzhou, Suzhou, Taizhou and Nantong in Jiangsu Province in December 2022. The concentrations of PAEs in the different samples were determined by gas chromatography-mass spectrometry. The main PAEs detected were bis(2-ethylhexyl) phthalate (DEHP), dibutyl phthalate (DBP), diisobutyl phthalate (DIBP), and di-n-octyl phthalate (DNOP). The total concentration ranges of PAEs in water, sediment, and soil were not from detected to 13 757 ng·L^-1, 78.4 to 2 618 μg·kg^-1, and 56.7 to 1 329 μg·kg^-1, respectively. The average PAEs concentrations in water, sediment, and soil were 1 369 ng·L^-1, 661 μg·kg^-1, and 442 μg·kg^-1, respectively. High concentrations of PAEs were detected in surface water and drinking water in Nantong and Taizhou, and in sewage treatment plant effluent in Taizhou. High concentrations of PAEs were also detected in soil and sediment in Nantong and Taizhou. The risk entropy method was used to assess the risk levels of the PAEs. The results show that PAEs in surface water, soil, and sediment in typical chemical parks in Jiangsu Province presented a moderate to high degree of risk. High risk was presented by PAEs in sewage treatment plants. A health risk evaluation show that the PAEs health risk entropy in drinking water and water sources around chemical industrial parks in Jiangsu Province ranged from 0 to 0.191 2. The PAEs in drinking water presented a moderate risk in Nantong and a low risk in other areas. Overall, samples from Nantong and Taizhou showed the highest levels of pollution and had risks that were above moderate levels; therefore, pollution in these areas should receive high attention. Further analysis is required to identify the sources of PAEs pollution in these areas so that effective measures can be taken to control excessive emission of such pollutants into the environment.

Key words: phthalate ester, chemical industry park, pollution characteristic, risk assessment

中图分类号:

X502
X503

古文, 汪贞, 梁梦园, 范德玲, 邢维龙, 孙帅, 张冰, 王蕾, 石利利. 江苏省典型化工园区7种邻苯二甲酸酯污染特征及风险评估[J]. 生态与农村环境学报, 2023, 39(11): 1504-1514.

GU Wen, WANG Zhen, LIANG Meng-yuan, FAN De-ling, XING Wei-long, SUN Shuai, ZHANG Bing, WANG Lei, SHI Li-li. Pollution Characteristics and Risk Assessment of Seven Phthalate Esters in Typical Chemical Industry Parks in Jiangsu Province[J]. Journal of Ecology and Rural Environment, 2023, 39(11): 1504-1514.

参考文献

[1] OLIVER R, MAY E, WILLIAMS J.Microcosm Investigations of Phthalate Behaviour in Sewage Treatment Biofilms[J].Science of the Total Environment, 2007, 372(2/3):605-614.
[2] 张焕云, 吴卓, 戴佳佳, 等.DINP皮肤暴露对小鼠过敏性皮肤炎症的佐剂作用[J].中国环境科学, 2015, 35(12):3804-3809.[ZHANG Huan-yun, WU Zhuo, DAI Jia-jia, et al.Adjuvant Effect of Skin DINP Exposure on Mice with Allergic Dermatitis[J].China Environmental Science, 2015, 35(12):3804-3809.]
[3] 朱冰清, 高占啟, 胡冠九, 等.太湖重点区域水环境中邻苯二甲酸酯的污染水平及生态风险评价[J].环境科学, 2018, 39(8):3614-3621.[ZHU Bing-qing, GAO Zhan-qi, HU Guan-jiu, et al.Contamination Levels and Ecological Risk Assessment of Phthalate Esters(PAEs) in the Aquatic Environment of Key Areas of Taihu Lake[J].Environmental Science, 2018, 39(8):3614-3621.]
[4] WORMUTH M, SCHERINGER M, VOLLENWEIDER M, et al.What Are the Sources of Exposure to Eight Frequently Used Phthalic Acid Esters in Europeans?[J].Risk Analysis, 2006, 26(3):803-824.
[5] 刘成, 孙翠竹, 张哿, 等.胶州湾表层水体中邻苯二甲酸酯的污染特征和生态风险[J].环境科学, 2019, 40(4):1726-1733.[LIU Cheng, SUN Cui-zhu, ZHANG Ge, et al.Pollution Characteristics and Ecological Risk Assessment of Phthalate Esters (PAEs) in the Surface Water of Jiaozhou Bay[J].Environmental Science, 2019, 40(4):1726-1733.]
[6] VAN WEZEL A P, VAN VLAARDINGEN P, POSTHUMUS R, et al.Environmental Risk Limits for Two Phthalates, with Special Emphasis on Endocrine Disruptive Properties[J].Ecotoxicology and Environmental Safety, 2000, 46(3):305-321.
[7] FUJII M, SHINOHARA N, LIM A, et al.A Study on Emission of Phthalate Esters from Plastic Materials Using a Passive Flux Sampler[J].Atmospheric Environment, 2003, 37(39/40):5495-5504.
[8] BECKER K, SEIWERT M, ANGERER J, et al.DEHP Metabolites in Urine of Children and DEHP in House Dust[J].International Journal of Hygiene and Environmental Health, 2004, 207(5):409-417.
[9] TAN G H.Residue Levels of Phthalate Esters in Water and Sediment Samples from the Klang River Basin[J].Bulletin of Environmental Contamination and Toxicology, 1995, 54(2):171-176.
[10] 周文敏, 傅德黔, 孙宗光.中国水中优先控制污染物黑名单的确定[J].环境科学研究, 1991, 4(6):9-12.[ZHOU Wen-min, FU De-qian, SUN Zong-guang.Determination of Black List of China's Priority Pollutants in Water[J].Research of Environmental Sciences, 1991, 4(6):9-12.]
[11] LUO M K, YU H, LIU Q, et al.Effect of River-lake Connectivity on Heavy Metal Diffusion and Source Identification of Heavy Metals in the Middle and Lower Reaches of the Yangtze River[J].Journal of Hazardous Materials, 2021, 416:125818.
[12] 胡雄星, 韩中豪, 周亚康, 等.黄浦江表层水体中邻苯二甲酸酯的分布特征及风险评价[J].环境化学, 2007, 26(2):258-259.[HU Xiong-xing, HAN Zhong-hao, ZHOU Ya-kang, et al.Distribution Characteristics and Risk Assessment of Phthalates in Surface Water of Huangpu River[J].Environmental Chemistry, 2007, 26(2):258-259.]
[13] 魏薇, 谢莹, 王建刚, 等.邻苯二甲酸酯在松花江吉林段水体中的分布规律[J].中国环境监测, 2011, 27(5):60-64.[WEI Wei, XIE Ying, WANG Jian-gang, et al.Distribution Law of PAEs in the Water Body of Songhua River Jilin Section[J].Environmental Monitoring in China, 2011, 27(5):60-64.]
[14] 董继元, 王式功, 尚可政.黄河兰州段邻苯二甲酸酯类有机污染物健康风险评价[J].农业环境科学学报, 2010, 29(5):963-968.[DONG Ji-yuan, WANG Shi-gong, SHANG Ke-zheng.Water Environmental Health Risk Assessment of Phthalic Acid Esters in Lanzhou Reach of Yellow River[J].Journal of Agro-environment Science, 2010, 29(5):963-968.]
[15] 卓丽, 石运刚, 蔡凤珊, 等.长江干流、嘉陵江和乌江重庆段邻苯二甲酸酯污染特征及生态风险评估[J].生态毒理学报, 2020, 15(3):158-170.[ZHUO Li, SHI Yun-gang, CAI Feng-shan, et al.Pollution Characteristics and Ecological Risk Assessment of Phthalate Esters in the Yangtze River, Jialing River and Wujiang River in Chongqing, China[J].Asian Journal of Ecotoxicology, 2020, 15(3):158-170.]
[16] VERLICCHI P, AL AUKIDY M, GALLETTI A, et al.Hospital Effluent:Investigation of the Concentrations and Distribution of Pharmaceuticals and Environmental Risk Assessment[J].Science of the Total Environment, 2012, 430:109-118.
[17] HE Y, SU S, LYU Y, et al.Occurrence of Methylsiloxanes in Sediments from a Subtropical River-lake System in Eastern China and Its Implication for Ecological Risks[J].Ecotoxicology and Environmental Safety, 2021, 223:112627.
[18] 方昊, 余军楠, 王智峰, 等.江苏典型中华绒螯蟹养殖区抗生素污染特征与生态风险评估[J].生态与农村环境学报, 2019, 35(11):1436-1444.[FANG Hao, YU Jun-nan, WANG Zhi-feng, et al.Contamination Characteristics and Ecological Risk Assessment of Antibiotics in Typical Eriocheir sinensis Aquaculture Environments of Jiangsu Province[J].Journal of Ecology and Rural Environment, 2019, 35(11):1436-1444.]
[19] 徐怀洲, 宋宁慧, 张圣虎, 等.骆马湖邻苯二甲酸酯分布特征及健康风险评价[J].生态与农村环境学报, 2017, 33(10):928-934.[XU Huai-zhou, SONG Ning-hui, ZHANG Sheng-hu, et al.Distribution Characteristics and Health Risk Assessment of Phthalate Esters in Lake Luoma[J].Journal of Ecology and Rural Environment, 2017, 33(10):928-934.]
[20] SHI W, ZHANG F X, ZHANG X W, et al.Identification of Trace Organic Pollutants in Freshwater Sources in Eastern China and Estimation of Their Associated Human Health Risks[J].Ecotoxicology, 2011, 20(5):1099-1106.
[21] HE H, HU G J, SUN C, et al.Trace Analysis of Persistent Toxic Substances in the Main Stream of Jiangsu Section of the Yangtze River, China[J].Environmental Science and Pollution Research International, 2011, 18(4):638-648.
[22] SHI W, HU X X, ZHANG F X, et al.Occurrence of Thyroid Hormone Activities in Drinking Water from Eastern China:Contributions of Phthalate Esters[J].Environmental Science & Technology, 2012, 46(3):1811-1818.
[23] AMIR S, HAFIDI M, MERLINA G, et al.Fate of Phthalic Acid Esters during Composting of both Lagooning and Activated Sludges[J].Process Biochemistry, 2005, 40(6):2183-2190.
[24] WANG J L, LIU P, QIAN Y.Biodegradation of Phthalic Acid Esters by Acclimated Activated Sludge[J].Environment International, 1996, 22(6):737-741.
[25] KONG M H, SONG Y H, ZHANG Y Z, et al.Fate of Phthalate Esters in Municipal Wastewater Treatment Plant and Their Environmental Impact[J].Water Science and Technology, 2016, 73(6):1395-1400.
[26] GAO D W, LI Z, WEN Z D, et al.Occurrence and Fate of Phthalate Esters in Full-scale Domestic Wastewater Treatment Plants and Their Impact on Receiving Waters along the Songhua River in China[J].Chemosphere, 2014, 95:24-32.
[27] 李梅, 王翠彦, 于小迪, 等.污水处理厂中邻苯二甲酸酯类物质分布及去除特性研究[J].安全与环境学报, 2014, 14(5):186-190.[LI Mei, WANG Cui-yan, YU Xiao-di, et al.Distribution and Removal Characteristics of Phthalic Acid Esters in Sewage Treatment Plants[J].Journal of Safety and Environment, 2014, 14(5):186-190.]
[28] 周林军, 古文, 刘济宁, 等.11种邻苯二甲酸酯在好氧污水处理系统中的归趋[J].环境科学, 2017, 38(5):1972-1981.[ZHOU Lin-jun, GU Wen, LIU Ji-ning, et al.Fate of Eleven Phthalic Acid Esters in Aerobic Sewage Treatment System[J].Environmental Science, 2017, 38(5):1972-1981.]
[29] TAN B L L, HAWKER D W, MüLLER J F, et al.Modelling of the Fate of Selected Endocrine Disruptors in a Municipal Wastewater Treatment Plant in South East Queensland, Australia[J].Chemosphere, 2007, 69(4):644-654.
[30] 国家环境保护总局, 国家质量监督检验检疫总局.地表水环境质量标准:GB 3838-2002[S].北京:中国环境科学出版社, 2002.
[31] LIU H, CUI K Y, ZENG F, et al.Occurrence and Distribution of Phthalate Esters in Riverine Sediments from the Pearl River Delta Region, South China[J].Marine Pollution Bulletin, 2014, 83(1):358-365.
[32] LIU H, LIANG H C, LIANG Y, et al.Distribution of Phthalate Esters in Alluvial Sediment:A Case Study at Jianghan Plain, Central China[J].Chemosphere, 2010, 78(4):382-388.
[33] SRIVASTAVA A, SHARMA V P, TRIPATHI R, et al.Occurrence of Phthalic Acid Esters in Gomti River Sediment, India[J].Environmental Monitoring and Assessment, 2010, 169(1/2/3/4):397-406.
[34] VITALI M, GUIDOTTI M, MACILENTI G, et al.Phthalate Esters in Freshwaters as Markers of Contamination Sources:A Site Study in Italy[J].Environment International, 1997, 23(3):337-347.
[35] 费勇, 陈江, 倪晓芳, 等.湖州地区土壤邻苯二甲酸酯空间分布现状特征分析[J].农业环境与发展, 2010, 27(2):83-86.[FEI Yong, CHEN Jiang, NI Xiao-fang, et al.Analysis on Spatial Distribution of Phthalate Esters in Huzhou Area[J].Agro-environment & Development, 2010, 27(2):83-86.]
[36] CARTWRIGHT C D, THOMPSON I P, BURNS R G.Degradation and Impact of Phthalate Plasticizers on Soil Microbial Communities[J].Environmental Toxicology and Chemistry, 2000, 19(5):1253-1261.
[37] 蔡全英, 莫测辉, 李云辉, 等.广州、深圳地区蔬菜生产基地土壤中邻苯二甲酸酯(PAEs)研究[J].生态学报, 2005, 25(2):283-288.[CAI Quan-ying, MO Ce-hui, LI Yun-hui, et al.The Study of PAEs in Soils from Typical Vegetable Fields in Areas of Guangzhou and Shenzhen, South China[J].Acta Ecologica Sinica, 2005, 25(2):283-288.]
[38] NORMAN.NORMAN Ecotoxicology Database:Lowest PNECs[EB/OL].[2023-03-22].https://www.norman-network.com/nds/ecotox/lowestPnecsIndex.php.
[39] European Chemicals Agency.REACH Registration Data[EB/OL].[2023-03-22].https://echa.europa.eu/home.
[40] US EPA.Integrated Risk Information System[EB/OL].[2023-03-22].https://www.epa.gov/iris.
[41] 王晓南, 张瑜, 王婉华, 等.邻苯二甲酸二乙基己酯(DEHP)污染及其毒性研究进展[J].生态毒理学报, 2017, 12(3):135-150.[WANG Xiao-nan, ZHANG Yu, WANG Wan-hua, et al.Environmental Pollution and Toxicity of DEHP[J].Asian Journal of Ecotoxicology, 2017, 12(3):135-150.]
[42] 丁梦雨, 康启越, 张释义, 等.全国23个城市水源水中邻苯二甲酸酯代谢物浓度调查[J].中国环境科学, 2019, 39(10):4205-4211.[DING Meng-yu, KANG Qi-yue, ZHANG Shi-yi, et al.National Survey of Phthalate Metabolites in Drinking Source Water of 23 Cities in China[J].China Environmental Science, 2019, 39(10):4205-4211.]