Abstract：Twenty-seven surface marine sediments were collected from Pearl River Estuary and adjacent waters in 2020 to evaluate the distribution characteristics and potential sources of polychlorinated biphenyls (PCBs). Thirty-seven PCB congeners and 10PCBs homologues including mono- to deca-PCBs were analyzed with isotope dilution HRGC/HRMS. The results show that:(1) the Σ37PCBs concentrations in the study area ranged from 0.024 to 5.11ng/g, with at least one target PCBs congeners being detected in the sediment, and was lower than that in near-shore coastal waters around the world; (2) the PCBs concentrations were higher in Zhuhai coastal waters and Humen outlet than in other study areas, particularly higher in the offshore areas, implying that they likely originated from land-based pollution sources; (3) PCB-11was the dominant compound observed in the surface sediments, with the highest detection frequency and a higher concentration than that of Σmarker PCBs; and (4) the traditional PCBs products were the main contributors to PCBs contamination only in the west coast of Shenzhen while the production and usage of diarylide yellow pigments could be the potential source of PCBs contamination in other study sites. Obviously, the contribution of marker-PCBs was limited to PCBs contamination in the PRD. Therefore, more attentions are required to control the contamination of non-Aroclor PCBs (such as PCB-11) to help regulate emerging contamintion in coastal marine environment of China.
Erickson M D, Kaley R G. Applications of polychlorinated biphenyls[J]. Environmental Science and Pollution Research, 2011,18(2):135-151.
[2]
Lauby-Secretan B, Loomis D, Grosse Y, et al. Carcinogenicity of polychlorinated biphenyls and polybrominated biphenyls[J]. The Lancet Oncolngy, 2013,14(4):287.
[3]
毕新慧,徐晓白.多氯联苯的环境行为[J].化学进展, 2000,12(2):152-160. Bi X H, Xu X B. Behaviors of PCBs in environment[J]. Progress in Chemistry, 2000,12(2):152-160.
[4]
Mai, B, Zeng, E Y, Luo, X, et al.Abundances, depositional fluxes, and homologue patterns of polychlorinated biphenyls in dated sediment cores from the Pearl River Delta, China[J]. Environment Sciece & Technology, 2005,39(1):49-56.
[5]
Li H, Ye S, Ye J, et al. Baseline survey of sediments and marine organisms in Liaohe estuary:Heavy metals, polychlorinated biphenyls and organochlorine pesticides[J]. Marine Pollution Bulletin, 2017, 114(1):555-563.
[6]
Hu D, Martinez A, Hornbuckle K C. Discovery of non-aroclor PCB (3, 3'-dichlorobiphenyl) in Chicago air[J]. Environment Sciece & Technology, 2008,42(21):7873-7877.
[7]
Liu G, Zheng M, Ba T, et al. A preliminary investigation on emission of polychlorinated dibenzo-p-dioxins/dibenzofurans and dioxin-like polychlorinated biphenyls from coke plants in China[J]. Chemosphere, 2009,75(5):692-695.
[8]
Shibamoto T, Yasuhara A, Katami T. Dioxin formation from waste incineration[J]. Reviews of Environmental Contamination and Toxicology, 2007,190:1-41.
[9]
Yuan D, Yang D, Wade T L, et al. Status of persistent organic pollutants in the sediment from several estuaries in China[J]. Environmental Pollution, 2001,114(1):101-111.
[10]
Kannan K, Johnson-Restrepo B, Yohn S S, et al. Spatial and temporal distribution of polycyclic aromatic hydrocarbons in sediments from Michigan inland lakes[J]. Environmental Science & Technology, 2005,39(13):4700-6.
[11]
Marvin C H, Painter S, Charltom M N, et al. Trends in spatial and temporal levels of persistent organic pollutants in Lake Erie sediments[J]. Chemosphere, 2004,54(1):33-40.
[12]
Guzzella L. PCBs and organochlorine pesticides in lake Orta (Northern Italy) sediments[J]. Water Air & Soil Pollution, 1997,99(1-4):245-254.
[13]
Iwata H, Tanabe S, Sakai N, et al. Geographical distribution of persistent organochlorines in air, water and sediments from Asia and Oceania, and their implications for global redistribution from lower latitudes[J]. Environmental Pollution, 1994,85(1):15-33.
[14]
Hong S H, Yim U H, Shim W J, et al. Congener-specific survey for polychlorinated biphenyls in sediments of industrialized bays in Korea:regional characteristics and pollution sources[J]. Environmental Science & Technology, 2005,39(19):7380-7388.
[15]
徐磊,刘莎,秦庆东,等.太湖竺山湾及入湖河流沉积物中多氯联苯单体分布及源解析[J].中国环境科学, 2017,37(11):4333-4341. Xu L, Liu S, Qin Q D, et al. Distribution and source apportionment of polychlorinated biphenyl congeners in surface sediments from Zhushan Bay and the inflow rivers of Lake Taihu[J]. China Environmental Science, 2017,37(11):4333-4341.
[16]
许妍,陈佳枫,徐磊,等.白洋淀表层沉积物中有机氯农药和全多氯联苯的分布特征及风险评估[J].湖泊科学, 2020,32(3):654-664. Xu Y, Chen J F, Xu L, et al. Distribution and risk assessment of organochlorine pesticides and polychlorinated biphenyls in surficial sediments from Lake Baiyangdian. J. Lake Sci. 2020,32(3):654-664.
[17]
赵颖,王飞,葛宜虎.汾河流域沉积物中多氯联苯的分布及生态风险评价[J].水资源保护, 2018,34(5):81-87. Zhao Y, Wang F, Ge Y H. Distribution of polychlorinated biphenyl in sediments of Fenhe River[J]. Water Resources Protection, 2018,34(5):81-87.
[18]
刘贝贝.深圳西部海域表层沉积物中多环芳烃和多氯联苯的污染特征及来源初探[D].湛江:广东海洋大学, 2015. Liu B B. The pollution characteristics and preliminary source apportionment of polycyclic aromatic hydrocarbons and polychlorinated biphenyls in surface sediments from the western sea of Shenzhen[D]. Zhan jiang:Guangdong Ocean University, 2015.
[19]
李光耀,金军,何畅,等.黄河表层沉积物中类二噁英多氯联苯水平分布[J].环境科学, 2014,35(9):3358-3364. Li G Y, Jin J, He C, et al. Levels and Distribution of the Dioxin-Like Polychlorinated Biphenyls (PCBs) in the Surface Sediment of the Yellow River[J]. Environmental Science, 2014,(9):3358-3364.
[20]
张岩,裴国霞,邰生霞,等.黄河内蒙古段头道拐断面沉积物中六六六(HCHs)和多氯联苯(PCBs)的残留特征分析研究[J].中国农村水利水电, 2011,(3):26-28. Zhang Y, Pei G X, Tai S X, et al. Investgation of HCHs and PCBs in the Sediments at the Toudaoguai Section of the Yellow River[J]. China Rural Water and Hydropower, 2011,(3):26-28.
[21]
康跃惠,盛国英,傅家谟,等.珠江三角洲一些表层沉积物中多氯联苯的初步研究[J].环境化学, 2000,19(3):262-269. Kang Y H, Sheng G Y, Fu J M, et al. Prelminary study on the distribution and characterization of polychlorinated biphenyls in some of surface sediments from Pearl River Delta[J]. Environmental Chemistry, 2000,19(3):262-269.
[22]
管玉峰,岳强,涂秀云,等.珠江入海口水体中多氯联苯的分布特征及其来源分析[J].环境科学研究, 2011,24(8):865-872. Guan Y F, Yue Q, Tu X Y, et al. Distribution and Sources of Polychlorinated Biphenyls (PCBs) in Riverine Water of the Outlets of the Pearl River Delta[J]. Research of Environmental Sciences, 2011, 24(8):865-872.
[23]
张蓬.渤黄海沉积物中的多环芳烃和多氯联苯及其与生态环境的耦合解析[D].青岛:中国科学院研究生院(海洋研究所), 2009. Zhang P. PAHs and PCBs biogeochemical characteritics in the sediments and coupling eith the eco-environments in the Bohai Sea and the Southern Yellow Sea.[D]. Qingdao:Institute of Oceanology, Chinese Academy of Sciences, 2009.
[24]
郭军辉,殷月芬,韩彬,等.莱州湾表层沉积物中多氯联苯的测定方法及分布特征探究[J].中国环境监测, 2011,27(3):35-41. Guo J H, Yin Y F, Han B, et al. The Determination Methods and the Exploring to the Distributional Characteristics of PCBs in Surface Sediments of Laizhou Bay[J]. Environmental Monitoring in China, 2011,27(3):35-41.
[25]
段晓勇.黄、东海沉积物中多氯联苯的分布及来源[D].青岛:中国海洋大学, 2014. Duan X Y. Distributions and sources of polychlorinated biphenyls in the Yellow Sea and the East China Sea inner shelf sediments[D]. Qingdao:Ocean University of China, 2014.
[26]
Liu W X, Chen J L, Hu J, et al. Multi-residues of organic pollutants in surface sediments from littoral areas of the Yellow Sea, China[J]. Marine Pollution Bulletin, 2008,56(6):1091-1103.
[27]
刘保良,陈旭阳,魏春雷,等.北海近岸海域表层沉积物中DDTs、PCBs的分布、来源与生态风险分析[J].广西科学, 2021,28(1):23-29. Liu B L, ChenX Y, Wei C L, et al. Distribution, sources and ecological risk analysis of DDTs and PCBs in surface sediments of Beihai Sea Coast[J]. Guangxi Sciences, 2020,28(1):23-29.
[28]
李源媛,王英辉,李平阳,等.钦州湾表层沉积物中多氯联苯的分布特征及风险评价[J].海洋环境科学, 2013,32(5):698-701. Li Y Y, Wang Y H, LI P Y, et al. Spatial distribution and risk assessment of polychlorinated biphenyl in surface sediments of Qinzhou Bay[J]. Marine Environmental Sciences, 2013,32(5):698-701.
[29]
黎晓霞,张珞平,蔡河山.厦门西海域拟疏浚物中多氯联苯含量分布及生态风险评价[J].环境监测管理与技术, 2008,20(6):30-32. Li X X, Zhang L P, Cai H S. Distribution of PCBs concentration in dredged materials of Xiamen Western Bay andecological hazard assessment[J]. The Administration and Technique of Environmental Monitoring, 2008,20(6):30-32.
[30]
夏佳玮.长江口及其邻近海域表层沉积物中多氯联苯的时空分布及其潜在生态风险评价研究[D].上海:上海海洋大学, 2017. Xia J W. Temporal and spatial distribution and potential risk assessment of polychlorinated biphenyls in surface sediments from the Changjiang Estuary and its adjacent areas[D]. Shanghai:Shanghai Ocean University, 2017.
[31]
章一帆,薛斌,周珊珊,等.福建兴化湾沉积物中多氯联苯的残留和风险评价[J].湖南科技大学学报(自然科学版), 2011,26(3):120-124. Zhang Y F, Xue B, Zhou S S, et al. Residues and risk assessment of polychlorinated biphenyls in sediments from Xinghua Bay in Fujian[J]. Journal of Hunan University of Science & Technology (Natural Science Edition), 2011,26(3):120-124.
[32]
梅卫平,阮慧慧,吴昊,等.滴水湖水系表层沉积物中多氯联苯残留与风险评价[J].中国环境科学, 2014,34(8):2086-2092. Mei W P, Ruan H H, Wu H, et al. Residual characteristics and ecological risk assessment of polychlorinated biphenyls (PCBs) in the surface[J]. China Environmental Science, 2014,34(8):2086-2092.
[33]
姜重臣.大亚湾海域有机污染物的来源及其分布特征研究.青岛:中国海洋大学, 2005. Jiang Z C. Sutdy on ogrnaie pollutants sources and their distribution charaeteristics in Daya Bay[D]. Qingdao:Ocean University of China, 2015.
[34]
陈思杨,宋琍琍,刘希真,等.浙江典型海湾潮间带沉积物污染及生态风险评价[J].中国环境科学, 2020,40(4):1771-1781. Chen S Y, Song L L, Liu X Z, et al. Evaluation on sediment pollution and potential ecological risks in the intertidal zone of typical bays in Zhejiang Province[J]. China Environmental Science, 2020,40(4):1771-1781.
[35]
Lao Q, Liu G, Zhou X, et al. Sources of polychlorinated biphenyls (PCBs) and dichlorodiphenyltrichloroethanes (DDTs) found in surface sediment from coastal areas of Beibu Gulf:A reflection on shipping activities and coastal industries[J]. Marine Pollution Bulletin, 2021, 167:112318.
[36]
Deng Z, Li X, Chen C, et al. Distribution characteristics and environmental fate of PCBs in marine sediments at different latitudinal regions:Insights from congener profiles[J]. Marine Pollution Bulletin, 2020,161(Part A).
[37]
Lai Z, Li X, Li H, et al. Residual Distribution and Risk Assessment of Polychlorinated Biphenyls in Surface Sediments of the Pearl River Delta, South China[J]. Bulletin of Environmental Contamination & Toxicology, 2015,(95):37-44.
[38]
GB 17378.3-2007海洋监测规范第3部分:样品采集、贮存与运输[S]. GB 17378.3-2007 The specification for marine monitoring Part 3:Sample collection, storage and transportation[S].
[39]
GB17378.5-2007海洋监测规范第5部分:沉积物分析[S]. GB17378.5-2007 The specification for marine monitoring-Part 5:Sediment analysis[S].
[40]
US EPA 1668C-2010, Chlorinated Biphenyl Congeners in Water, Soil, Sediment, Biosolids, and Tissue by HRGC/HRMS[S].
Wang P, Shang H, Li H, et al. PBDEs, PCBs and PCDD/Fs in the sediments from seven major river basins in China:Occurrence, congener profile and spatial tendency[J]. Chemosphere, 2016,144(FEB.):13-20.
[43]
杨华云.长江三角洲毗邻海域有机氯农药和多氯联苯的研究[D].杭州:浙江工业大学, 2011. Yang H Y. Study on organochlorine pesticices and Polychlorinated Biphenyls in Yangtze River Delta and adjacent sea[D]. Hangzhou:Zhejiang University of Technology, 2011.
[44]
赵宾峰,祝翔宇,廖一波,等.象山港沉积物与生物体中多氯联苯分布特征与暴露风险[J].环境化学, 2020,39(10):2742-2752. Zhao B F, Zhu X Y, Liao Y B, et al. Distribution features and exposure risk of polychlorinated biphenyls (PCBs) in sediments and marine organisms from Xiangshan Bay, China[J]. Environmental Chemistry, 2020,39(10):2742-2752.
[45]
王江涛,谭丽菊,张文浩,等.青岛近海沉积物中多环芳烃、多氯联苯和有机氯农药的含量和分布特征[J].环境科学, 2010,31(11):2713-2722. Wang J T, Tan L J, Zhang W H, et al. Concentrations and distribution characteristic of PAHs, PCBs and OCPs in the surface sediments of Qingtao Coastal Area[J]. Environmental Science, 2010,31(11):2713-2722.
[46]
郭军辉,殷月芬,郑立,等.胶州湾东岸表层沉积物中多氯联苯的分布特征及风险评价[J].农业环境科学学报, 2011,30(5):965-972. Guo J H, Yin Y F, Zheng L, et al. The Distribution and Risk Assessment of Polychlorinated biphenyl in Surface Sediments in Estuaries of Jiaozhou Bay, China[J]. Journal of Agro-Environment Science, 2011,30(5):965-972.
[47]
Kannan V M, Gopikrishna V G, Saritha V K, et al. PCDD/Fs, dioxin-like, and non-dioxin like PCBs in the sediments of high Arctic fjords, Svalbard[J]. Marine pollution bulletin, 2022(Jan.):174.
[48]
薛斌.南极普里兹湾和南极半岛附近海域沉积物中典型持久性污染物的残留特征和来源解析[D].武汉:中国地质大学, 2014. Xue B. The distribution and source of typical persistent pollutants in surface sediments of Prydz Bay and Peninsula, Antarctic[D]. Wuhan:China University of Geosciences, 2014.
[49]
Bersuder P, Smith A J, Hynes C, et al. Baseline survey of marine sediments collected from the Kingdom of Bahrain:PAHs, PCBs, organochlorine pesticides, perfluoroalkyl substances, dioxins, brominated flame retardants and metal contamination[J]. Marine Pollution Bulletin, 2020,161:111734.
[50]
Neira C, Vales M, Mendoza G, et al. Polychlorinated biphenyls (PCBs) in recreational marina sediments of San Diego Bay, southern California[J]. Marine Pollution Bulletin, 2018,126(JAN.):204-214.
[51]
Jafarabadi A R, Bakhtiari A R, Mitraet S, et al. First polychlorinated biphenyls (PCBs) monitoring in seawater, surface sediments and marine fish communities of the Persian Gulf:Distribution, levels, congener profile and health risk assessment-ScienceDirect[J]. Environmental Pollution, 2019,253:78-88.
[52]
Lyons B P, Barber J L, Rumney H S, et al. Baseline survey of marine sediments collected from the State of Kuwait:PAHs, PCBs, brominated flame retardants and metal contamination[J]. Marine Pollution Bulletin, 2015,100(2):629-636.
[53]
Gedik K, Demircioglu F, Imamoglu I. Spatial distribution and source apportionment of PCBs in sediments around zmit industrial complexes, Turkey[J]. Chemosphere, 2010,81(8):992-999.
[54]
杨丹丹.渤海表层沉积物中多氯联苯(PCBs)的分布、来源及风险研究[D].青岛:中国海洋大学, 2015. Yang D D. Distribution,sources and risk research of Polychlorinated biphenyls (PCBs) in surface sediments of Bohai Sea.[D]. Qingdao:Ocean University of China, 2015.
[55]
Tang D, Liu X, He H, et al. Distribution, sources and ecological risks of organochlorine compounds (DDTs, HCHs and PCBs) in surface sediments from the Pearl River Estuary, China[J]. Marine Pollution Bulletin, 2020,152:110942.
[56]
Camacho-Ibar V F, McEvoy J. Total PCBs in Liverpool Bay sediments[J]. Marine Environmental Research, 1996,41:241-263.
[57]
Guerra R, Pasteris A, Lee S, et al. Spatial patterns of metals, PCDDs/Fs, PCBs, PBDEs and chemical status of sediments from a coastal lagoon (Pialassa Baiona, NW Adriatic, Italy)-ScienceDirect[J]. Marine Pollution Bulletin, 2014,89(1/2):407-416.
[58]
Zhang L H. Determination of PCBs content of transformer oil in Liaoning Power System[J]. Environmental Monitoring in China, 2008,24(3):23-25.
[59]
Breivik K, Sweetman A, Pacyna J M, et al. Towards a global historical emission inventory for selected PCB congeners-A mass balance approach:1. Global production and consumption[J]. Science of The Total Environment, 2002,290(1-3):181-198.
[60]
张志,齐虹,刘丽艳,等.中国生产的多氯联苯(PCBs)组分特征[J].黑龙江大学自然科学学报, 2009,26(6):809-815. Zhang Z, Qi H, Liu L Y, et al. Congener and homologue profiles of Polychlorinated Biphenyls (PCBs) produced in China.[J]. Journal of Natural Science of Heilongjiang University, 2009,26(6):809-815.
[61]
Schulz D E. Complete characterization of polychlorinated biphenyl congeners in commercial Aroclor and Clophen mixtures by multidimensional gas chromatography-electron capture detection[J]. Environment Sciece & Technology, 1989,23(7):852-859.
[62]
Litten S, Fowler B, Luszniak D. Identification of a novel PCB source through analysis of 209PCB congeners by US EPA modified method 1668[J]. Chemosphere, 2002,46(9/10):1457-1459.
[63]
Rodenburg L A, Guo J, Du S, et al. Evidence for unique and ubiquitous environmental sources of 3,3'-dichlorobiphenyl (PCB 11)[J]. Environmental Science & Technology, 2010,44(8):2816-2821.
[64]
Shang H, Li Y, Wang T, et al. The presence of polychlorinated biphenyls in yellow pigment products in China with emphasis on 3,3'-dichlorobiphenyl (PCB 11)[J]. Chemosphere, 2014,98:44-50.
[65]
King T L, Yeats P, Hellou J. Tracing the source of 3,3'-dichlorobiphenyl found in samples collected in and around Halifax Harbour[J]. Marine Pollution Bulletin, 2002,44(7):590-596.
[66]
Pizzini S, Sbicego C, Corami F, et al. 3,3'-dichlorobiphenyl (non-Aroclor PCB-11) as a marker of non-legacy PCB contamination in marine species:comparison between Antarctic and Mediterranean bivalves[J]. Chemosphere, 2017,175:28-35.
[67]
闫满宁,张合杰.上海捷虹颜料化工集团股份有限公司.黄色偶氮颜料环保生产的研究[J].上海染料, 2011,39(5):52-54. Yan M N, Zhang H J, Shanghai JECO. Reduce COD and Cost in the Yellow Pigment Production[J]. Shanghai Dyestuffs, 2011,39(5):52-54.
[68]
Shain W, Bush B, Seegal R. Neurotoxicity of polychlorinated biphenyls:structure-activity relationship of individual congeners[J]. Toxicol Appl Pharmacol, 1991,111(1):33-42.
[69]
Kodavanti P R S. Neurotoxicity of persistent organic pollutants:Possible mode (S) of action and further considerations[J]. Dose-Response, 2005,3(3):273-305.
[70]
Sethi S, Keil K P, Chen H, et al. Detection of 3,3'-Dichlorobiphenyl in Human Maternal Plasma and Its Effects on Axonal and Dendritic Growth in Primary Rat Neurons[J]. Toxicological Sciences, 2017, 158(2):401-411.
