华南地区典型食用鱼中4类卤代芳香化合物的污染特征和摄入风险
Pollution Characteristics and Intake Risks of Four Groups of Halogenated Aromatic Compounds in Representative Edible Fish from South China
-
摘要: 卤代芳香类化合物(HACs)具有环境普遍存在性、持久性、生物富集性和各种毒性，其污染和风险因此受到广泛关注。本研究对华南地区5种常见鱼肉中4类典型HACs进行了分析，结果表明，鱼肉中多氯代二苯并二噁英/呋喃(PCDD/Fs)、类二噁英多氯联苯(DL-PCBs)、多溴代二苯并二噁英/呋喃(PBDD/Fs)和总二噁英类(dioxins)毒性当量(TEQ)的平均值±标准偏差(范围)分别为(0.0680±0.3230) pg·g-1 (0～2.21 pg·g-1)、(0.118±0.124) pg·g-1 (0.000451～0.528 pg·g-1)、(0.139±0.164) pg·g-1 (0.00882～0.917 pg·g-1)和(0.325±0.366) pg·g-1 (0.0409～2.30 pg·g-1) (以单位湿质量计)，均低于欧盟规定的鱼肉中dioxins的TEQ限值；5种鱼中桂花鱼的总TEQ和摄入风险最高，其次是鳗鱼和鲶鱼，鲈鱼最低，但种类间并无显著差异。鱼肉中多溴联苯醚(PBDEs)的浓度(0.347±0.297) ng·g-1 (0.0191～1.40 ng·g-1) (以单位湿质量计)与国内外相比中等偏低，种类变化顺序为三文鱼＞鳗鱼＞鲈鱼＞桂花鱼＞鲶鱼。鱼肉中的PCDD/Fs以高氯代PCDDs为主，可能源于污染饲料和五氯酚/五氯酚钠的使用；DL-PCBs以PCB-118和PCB-105为主，主要源于其商业品和金属冶炼过程；PBDEs的来源包括其商业品和高溴PBDEs脱溴降解；PBDD/Fs以高溴PBDFs为主，其污染与PBDEs密切相关。华南地区居民通过膳食鱼肉摄入4类HACs的致癌和非致癌风险值分别为6.56×10-6～2.87×10-5和0.0314～0.114，其中儿童风险值高于青少年和成人。PBDD/Fs对总TEQ和摄入风险的贡献(平均45.6%)远高于其他HACs，其生物体污染和风险值得持续关注。Abstract: Halogenated aromatic compounds (HACs) exhibit environmental ubiquity, persistence, bioaccumulation, and diverse toxic effects, prompting widespread concern about their pollution and potential risks. This study investigated four categories of typical HACs in fish samples from five common species in South China. Results showed that the mean±standard deviation (range) of toxic equivalent quantity (TEQ) of polychlorinated dibenzo-p-dioxins/furans (PCDD/Fs), dioxins-like polychlorinated biphenyls (DL-PCBs), polybrominated dibenzo-p-dioxins/furans (PBDD/Fs), and total dioxins (dioxins) were (0.0680±0.3230) pg·g-1 (0～2.21 pg·g-1), (0.118±0.124) pg·g-1 (0.000451～0.528 pg·g-1), (0.139±0.164) pg·g-1 (0.00882～0.917 pg·g-1), and (0.325±0.366) pg·g-1 (0.0409～2.30 pg·g-1) (based on wet weight), respectively. All values were below the specified TEQ limit set by the European Union (EU) for dioxins in fish. Among the five fish species, mandarin fish exhibited the highest total TEQ and intake risk, followed by eel and catfish, while perch had the lowest. However, no statistical differences were observed in the TEQ among these five fish species. In comparison to global data, the concentrations of polybromodiphenyl ethers (PBDEs) in these fish samples (0.347±0.297) ng·g-1 (0.0191～1.40 ng·g-1) (based on wet weight) were at moderate or low levels with a changing trend among species: salmon>eel>perch>mandarin fish>catfish. The PCDD/Fs in these fish samples were predominantly high-chlorinated, possibly originating from PCDD/Fs-polluted feed and the use of pentachlorophenol/pentachlorophenol sodium. PCB-118 and PCB-105 were the dominant congeners of DL-PCBs in these samples, primarily sourced from commercial PCB products and various metal smelting processes. The sources of PBDEs in these fishes included commercial PBDE mixtures and the debromination of high-brominated PBDEs. PBDD/Fs showed dominance in high-brominated PBDFs, and their pollution was closely associated with PBDEs. The intake carcinogenic and non-carcinogenic risk values of these four HACs via fish consumption ranged from 6.56×10-6 to 2.87×10-5 and 0.0314 to 0.114, respectively, for the residents from South China, with higher values for children compared to teenagers and adults. PBDD/Fs contributed significantly higher total TEQ and intake risks (45.6% on average) than the other HACs, emphasizing the ongoing need for continuous attention to their pollution in biota and associated risks.
-
-
Ssebugere P, Sillanpää M, Matovu H, et al. Human and environmental exposure to PCDD/Fs and dioxin-like PCBs in Africa: A review [J]. Chemosphere, 2019, 223: 483-493 Bjurlid F, Roos A, Ericson Jogsten I, et al. Temporal trends of PBDD/Fs, PCDD/Fs, PBDEs and PCBs in ringed seals from the Baltic Sea (Pusa hispida botnica) between 1974 and 2015[J]. The Science of the Total Environment, 2018, 616/617: 1374-1383 Ohoro C R, Adeniji A O, Okoh A I, et al. Polybrominated diphenyl ethers in the environmental systems: A review [J]. Journal of Environmental Health Science & Engineering, 2021, 19(1): 1229-1247 Ceci R, Diletti G, Bellocci M, et al. Brominated and chlorinated contaminants in food (PCDD/Fs, PCBs, PBDD/Fs PBDEs): Simultaneous determination and occurrence in Italian produce [J]. Chemosphere, 2022, 288(Pt 1): 132445 Jiang Y F, Yuan L M, Lin Q H, et al. Polybrominated diphenyl ethers in the environment and human external and internal exposure in China: A review [J]. The Science of the Total Environment, 2019, 696: 133902 蒋友胜, 张建清, 周健, 等. 鱼体中二恶英、多氯联苯和多溴联苯醚的污染分析[J]. 中国卫生检验杂志, 2010, 20(7): 1631-1635 Jiang Y S, Zhang J Q, Zhou J, et al. Analyzed of PCDD/Fs, PCBs and PBDEs in fish sample [J]. Chinese Journal of Health Laboratory Technology, 2010, 20(7): 1631-1635(in Chinese)
Song A M, Li H R, Liu M Y, et al. Polybrominated dibenzo-p-dioxins/furans (PBDD/Fs) in soil around municipal solid waste incinerator: A comparison with polychlorinated dibenzo-p-dioxins/furans (PCDD/Fs) [J]. Environmental Pollution, 2022, 293: 118563 Falandysz J, Smith F, Fernandes A R. Polybrominated dibenzo-p-dioxins (PBDDs) and -dibenzofurans (PBDFs) in cod (Gadus morhua) liver-derived products from 1972 to 2017[J]. The Science of the Total Environment, 2020, 722: 137840 Liu M Y, Li H R, Song A M, et al. Polybrominated dibenzo-p-dioxins/furans and their chlorinated analogues in sediments from a historical hotspot for both brominated flame retardants and organochlorine pesticides [J]. Environmental Pollution, 2023, 316(Pt 1): 120489 Fernandes A R, Falandysz J. Polybrominated dibenzo-p-dioxins and furans (PBDD/Fs): Contamination in food, humans and dietary exposure [J]. The Science of the Total Environment, 2021, 761: 143191 Zhu M H, Yuan Y B, Yin H, et al. Environmental contamination and human exposure of polychlorinated biphenyls (PCBs) in China: A review [J]. The Science of the Total Environment, 2022, 805: 150270 Li C Q, Liu G R, Qin S, et al. Emission reduction of PCDD/Fs by flue gas recirculation and activated carbon in the iron ore sintering [J]. Environmental Pollution, 2023, 327: 121520 Sindiku O, Babayemi J O, Tysklind M, et al. Polybrominated dibenzo-p-dioxins and dibenzofurans (PBDD/Fs) in e-waste plastic in Nigeria [J]. Environmental Science and Pollution Research, 2015, 22(19): 14515-14529 Ebert J, Bahadir M. Formation of PBDD/F from flame-retarded plastic materials under thermal stress [J]. Environment International, 2003, 29(6): 711-716 Roszko M, Szymczyk K, Jędrzejczak R. Influence of hen breeding type on PCDD/F, PCB & PBDE levels in eggs [J]. The Science of the Total Environment, 2014, 487: 279-289 国家统计局. 中国统计年鉴1999[M/OL]. [2024-01-11 ]. https://www.stats.gov.cn/
国家统计局. 中国统计年鉴2020[M/OL]. [2024-01-11 ]. https://www.stats.gov.cn/
Pius C, Koosaletse-Mswela P, Dikinya O, et al. Polychlorinated dibenzo-p-dioxin/dibenzofurans (PCDD/Fs) contamination in sediments and fish from Msimbazi River in Dar es Salam, Tanzania: Patterns, sources, and their exposure to humans [J]. Environmental Monitoring and Assessment, 2023, 195(6): 631 Mikolajczyk S, Warenik-Bany M, Pajurek M. PCDD/Fs and PCBs in Baltic fish: Recent data, risk for consumers [J]. Marine Pollution Bulletin, 2021, 171: 112763 Zhang X M, Gandhi N, Bhavsar S P. Persistent organohalogens in paired fish fillet and eggs: Implications for fish consumption advisories [J]. Journal of Agricultural and Food Chemistry, 2016, 64(14): 2832-2840 Polak-Juszczak L, Waszak I, Szlinder-Richert J, et al. Levels, time trends, and distribution of dioxins and polychlorinated biphenyls in fishes from the Baltic Sea [J]. Chemosphere, 2022, 306: 135614 Li C, Yang L L, Shi M W, et al. Persistent organic pollutants in typical lake ecosystems [J]. Ecotoxicology and Environmental Safety, 2019, 180: 668-678 李玉芳, 宋淑玲. 中国主要沿海地区鱼/贝类中PBDEs暴露水平现状、特征和发展趋势[J]. 环境化学, 2020, 39(1): 138-147 Li Y F, Song S L. Current status, characteristics and development trend of PBDEs levels in fish/shellfish from major coastal areas of China [J]. Environmental Chemistry, 2020, 39(1): 138-147(in Chinese)
郭英, 唐洪磊, 孟祥周, 等. 多溴联苯醚在桂花鱼体内的分布[J]. 环境科学, 2007, 28(12): 2806-2810 Guo Y, Tang H L, Meng X Z, et al. Tissue distribution of PBDEs in mandarin fish [J]. Environmental Science, 2007, 28(12): 2806-2810(in Chinese)
管玉峰, 涂秀云, 吴宏海. 珠江入海口水体中多溴联苯醚及其来源分析[J]. 生态环境学报, 2011, 20(3): 474-479 Guan Y F, Tu X Y, Wu H H. Distribution and source of polybrominated diphenyl ethers (PBDEs) in riverine water of the Pearl River Delta [J]. Ecology and Environmental Sciences, 2011, 20(3): 474-479(in Chinese)
United States Environmental Protection Agency (US EPA). Tetra-through octa-chlorinated dioxins and furans by isotope dilution HRCC/HRMS [S]. Washington DC: Office of Water, 1994 United States Environmental Protection Agency (US EPA). Chlorinated biphenyl congeners in water, soil, sediment, biosolids, and tissue by HRCC/HRMS [S]. Washington DC: Office of Water, Office of Science and Technology, 2010 United States Environmental Protection Agency (US EPA). Brominated diphenyl ethers in water, soil, sediment and tissue by HRCC/HRMS [S]. Washington DC: Office of Water, Office of Science and Technology, 2007 周林, 李会茹, 马盛幍, 等. 土壤中PCDD/Fs、PBDD/Fs、PCBs与PBDEs同步分离测试方法的研究[J]. 分析测试学报, 2013, 32(10): 1160-1165 Zhou L, Li H R, Ma S T, et al. Simultaneous separation and determination of PCDD/Fs, PBDD/Fs, PCBs and PBDEs soil sample [J]. Journal of Instrumental Analysis, 2013, 32(10): 1160-1165(in Chinese)
van den Berg M, Birnbaum L S, Denison M, et al. The 2005 World Health Organization reevaluation of human and mammalian toxic equivalency factors for dioxins and dioxin-like compounds [J]. Toxicological Sciences: An Official Journal of the Society of Toxicology, 2006, 93(2): 223-241 van den Berg M, Denison M S, Birnbaum L S, et al. Polybrominated dibenzo-p-dioxins, dibenzofurans, and biphenyls: Inclusion in the toxicity equivalency factor concept for dioxin-like compounds [J]. Toxicological Sciences: An Official Journal of the Society of Toxicology, 2013, 133(2): 197-208 国家卫生健康委. 中国居民营养与慢性病状况报告-2020年[M]. 北京: 人民卫生出版社, 2021: 12-32 United States Environmental Protection Agency (US EPA). Technical fact sheet: Polybrominated diphenyl ethers (PBDEs) [R]. Washington DC: US EPA, 2017 Chiesa L M, Zanardi E, Nobile M, et al. Food risk characterization from exposure to persistent organic pollutants and metals contaminating eels from an Italian Lake [J]. Food Additives & Contaminants Part A, Chemistry, Analysis, Control, Exposure & Risk Assessment, 2019, 36(5): 779-788 Sprague M, Walton J, Campbell P J, et al. Replacement of fish oil with a DHA-rich algal meal derived from Schizochytrium sp. on the fatty acid and persistent organic pollutant levels in diets and flesh of Atlantic salmon (Salmo salar, L.) post-smolts [J]. Food Chemistry, 2015, 185: 413-421 Kljaković-Gašpić Z, Dvoršćak M, Orct T, et al. Metal(loid)s and persistent organic pollutants in yellow European eel from the Raša River, Croatia [J]. Marine Pollution Bulletin, 2023, 187: 114527 Rose M, Fernandes A, Mortimer D, et al. Contamination of fish in UK fresh water systems: Risk assessment for human consumption [J]. Chemosphere, 2015, 122: 183-189 Lupton S J, Ochoa C, Domesle A, et al. Survey of polychlorinated dibenzo-p-dioxins, polychlorinated dibenzofurans and non-ortho-polychlorinated biphenyls in U.S. meat, poultry, and siluriform fish from 2018-2019: Toxic equivalency levels, temporal trends, and implications [J]. Food Additives & Contaminants Part A, Chemistry, Analysis, Control, Exposure & Risk Assessment, 2022, 39(3): 560-571 Zacs D, Rjabova J, Fernandes A, et al. Brominated, chlorinated and mixed brominated/chlorinated persistent organic pollutants in European eels (Anquilla anquilla) from Latvian Lakes [J]. Food Additives & Contaminants Part A, Chemistry, Analysis, Control, Exposure & Risk Assessment, 2016, 33(3): 460-472 Zacs D, Rjabova J, Bartkevics V. Occurrence of brominated persistent organic pollutants (PBDD/DFs, PXDD/DFs, and PBDEs) in Baltic wild salmon (Salmo salar) and correlation with PCDD/DFs and PCBs [J]. Environmental Science & Technology, 2013, 47(16): 9478-9486 Struciński P, Piskorska-Pliszczyńska J, Maszewski S, et al. PCDD/Fs and DL-PCBs intake from fish caught in Polish fishing grounds in the Baltic Sea: Characterizing the risk for consumers [J]. Environment International, 2013, 56: 32-41 Jensen I J, Eilertsen K E, Otnæs C H A, et al. An update on the content of fatty acids, dioxins, PCBs and heavy metals in farmed, escaped and wild Atlantic salmon (Salmo salar L.) in Norway [J]. Foods, 2020, 9(12): 1901 Zhou Y X, Liu J S. Emissions, environmental levels, sources, formation pathways, and analysis of polybrominated dibenzo-p-dioxins and dibenzofurans: A review [J]. Environmental Science and Pollution Research International, 2018, 25(33): 33082-33102 Fernandes A R, Mortimer D, Holmes M, et al. Occurrence and spatial distribution of chemical contaminants in edible fish species collected from UK and proximate marine waters [J]. Environment International, 2018, 114: 219-230 Bramwell L, Mortimer D, Rose M, et al. UK dietary exposure to PCDD/Fs, PCBs, PBDD/Fs, PBBs and PBDEs: Comparison of results from 24-h duplicate diets and total diet studies [J]. Food Additives & Contaminants Part A, Chemistry, Analysis, Control, Exposure & Risk Assessment, 2017, 34(1): 65-77 Wang H S, Du J, Ho K L, et al. Exposure of Hong Kong residents to PBDEs and their structural analogues through market fish consumption [J]. Journal of Hazardous Materials, 2011, 192(1): 374-380 Voorspoels S, Covaci A, Neels H, et al. Dietary PBDE intake: A market-basket study in Belgium [J]. Environment International, 2007, 33(1): 93-97 Schecter A, Colacino J, Patel K, et al. Polybrominated diphenyl ether levels in foodstuffs collected from three locations from the United States [J]. Toxicology and Applied Pharmacology, 2010, 243(2): 217-224 Gebbink W A, van der Lee M K, Peters R J B, et al. Brominated flame retardants in animal derived foods in the Netherlands between 2009 and 2014[J]. Chemosphere, 2019, 234: 171-178 Li H R, Liu M Y, Hu J J, et al. Occurrence and carcinogenic potential of airborne PBDD/Fs and PCDD/Fs around a large-scale municipal solid waste incinerator: A long-term passive air sampling study [J]. Environment International, 2023, 178: 108104 Piskorska-Pliszczynska J, Strucinski P, Mikolajczyk S, et al. Pentachlorophenol from an old henhouse as a dioxin source in eggs and related human exposure [J]. Environmental Pollution, 2016, 208(Pt B): 404-412 Wang L Y, Ding G D, Zhou Z G, et al. Level and characteristics of polychlorinated dibenzo-p-dioxins and dibenzofurans in feed and feed additives [J]. Journal of Environmental Sciences (China), 2017, 51: 324-331 Ssebugere P, Sillanpää M, Wang P, et al. Polychlorinated biphenyls in sediments and fish species from the Murchison Bay of Lake Victoria, Uganda [J]. Science of the Total Environment, 2014, 482/483: 349-357 Rushneck D R, Beliveau A, Fowler B, et al. Concentrations of dioxin-like PCB congeners in unweathered Aroclors by HRGC/HRMS using EPA Method 1668A [J]. Chemosphere, 2004, 54(1): 79-87 Shen J, Yang L L, Yang Q T, et al. Polychlorinated biphenyl emissions from steelmaking electric arc furnaces [J]. Bulletin of Environmental Contamination and Toxicology, 2021, 106(4): 670-675 Wang M J, Hou M F, Zhao K, et al. Removal of polychlorinated biphenyls by desulfurization and emissions of polychlorinated biphenyls from sintering plants [J]. Environmental Science and Pollution Research International, 2016, 23(8): 7369-7375 Bjurlid F, Dam M, Hoydal K, et al. Occurrence of polybrominated dibenzo-p-dioxins, dibenzofurans (PBDD/Fs) and polybrominated diphenyl ethers (PBDEs) in pilot whales (Globicephala melas) caught around the Faroe Islands [J]. Chemosphere, 2018, 195: 11-20 Roszko M, Szymczyk K, Rzepkowska M, et al. Preliminary study on brominated dioxins/furans and hydroxylated/methoxylated PBDEs in Baltic cod (Gadus morhua) liver. Comparison to the levels of analogue chlorinated co-occurring pollutants [J]. Marine Pollution Bulletin, 2015, 96(1/2): 165-175 Bjurlid F, Kärrman A, Ricklund N, et al. Occurrence of brominated dioxins in a study using various firefighting methods [J]. The Science of the Total Environment, 2017, 599/600: 1213-1221 Xiao X, Hu J F, Peng P A, et al. Characterization of polybrominated dibenzo-p-dioxins and dibenzo-furans (PBDDs/Fs) in environmental matrices from an intensive electronic waste recycling site, South China [J]. Environmental Pollution, 2016, 212: 464-471 Hanari N, Kannan K, Miyake Y, et al. Occurrence of polybrominated biphenyls, polybrominated dibenzo-p-dioxins, and polybrominated dibenzofurans as impurities in commercial polybrominated diphenyl ether mixtures [J]. Environmental Science & Technology, 2006, 40(14): 4400-4405 Wyrzykowska-Ceradini B, Gullett B K, Tabor D, et al. PBDDs/Fs and PCDDs/Fs in the raw and clean flue gas during steady state and transient operation of a municipal waste combustor [J]. Environmental Science & Technology, 2011, 45(13): 5853-5860 Lv M C, Tang X X, Zhao Y R, et al. The toxicity, bioaccumulation and debromination of BDE-47 and BDE-209 in Chlorella sp. under multiple exposure modes [J]. The Science of the Total Environment, 2020, 723: 138086 Miyake Y, Jiang Q T, Yuan W, et al. Preliminary health risk assessment for polybrominated diphenyl ethers and polybrominated dibenzo-p-dioxins/furans in seafood from Guangzhou and Zhoushan, China [J]. Marine Pollution Bulletin, 2008, 57(6/12): 357-364 Chang J W, Hung C F, Hsu Y C, et al. Polybrominated diphenyl ethers (PBDES) and hexa-brominated biphenyls (Hexa-BBs) in fresh foods ingested in Taiwan [J]. Environmental Pollution, 2017, 220: 1180-1189 -
点击查看大图
计量
- 文章访问数: 918
- HTML全文浏览数: 918
- PDF下载数: 131
- 施引文献: 0
下载:
