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Spatial and temporal distributions of hexabromocyclododecanes in surface soils of Jinan, China

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Abstract

Contamination by hexabromocyclododecanes (HBCDDs) in the soil environment is an ongoing concern because of their “specific exemption” on the production and use in China. In this study, spatial distribution, temporal trend, and diastereoisomer profiles of HBCDDs were examined in surface soils collected in Jinan, China. Concentrations of ΣHBCDD (sum of α-, β-, and γ-HBCDDs) in soils ranged from 1.70 to 228 ng/g dry weight (dw), with a mean value of 26.1 ng/g dw. Soils collected from e-waste dismantling sites (mean 146 ng/g dw) contained significantly higher concentrations of ΣHBCDD than those of urban (15.5 ng/g dw) and farmland soils (3.86 ng/g dw) (p < 0.01). The temporal trend suggested that ΣHBCDD levels in the industrial area rose significantly between 2014 and 2019 (p < 0.05), with an annual increase of 12%. An increase in ΣHBCDD levels was also observed in urban and farmland soil samples during the study period, although it did not reach a significant level (p > 0.05). All surface soils were dominated by γ-HBCDD (mean 60.7% of total concentrations); however, the proportions of α-isomer increased from 28.7% in urban and rural soils to 43.4% in industrial soils. The calculated risk quotients of HBCDDs present in soils were at least 25-fold lower than the threshold limit value. The mean mass inventory of HBCDDs was approximately 2501 kg in the cultivated land of Jinan City; further studies are needed to discern the uptake of HBCDDs by crops and the fate of these chemicals in agricultural ecosystems.

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The datasets used and/or analyzed during the current study are available from the corresponding author on reasonable request.

References

  • Braune, B. M., Letcher, R. J., Gaston, A. J., & Mallory, M. L. (2015). Trends of polybrominated diphenyl ethers and hexabromocyclododecane in eggs of Canadian Arctic seabirds reflect changing use patterns. Environmental Research, 142, 651–661.

    CAS  Google Scholar 

  • Cao, X., Lu, Y., Zhang, Y., Khan, K., Wang, C., & Baninla, Y. (2018). An overview of hexabromocyclododecane (HBCDDs) in environmental media with focus on their potential risk and management in China. Environmental Pollution, 236, 283–295.

    CAS  Google Scholar 

  • Covaci, A., Gerecke, A. C., Law, R. J., Voorspoels, S., Kohler, M., Heeb, N. V., Leslie, H., Allchin, C. R., & Boer, J.d. (2006). Hexabromocyclododecanes (HBCDDs) in the environment and humans: a review. Environmental Science & Technology, 40, 3679–3688.

  • Drage, D., Mueller, J. F., Birch, G., Eaglesham, G., Hearn, L. K., & Harrad, S. (2015). Historical trends of PBDEs and HBCDDs in sediment cores from Sydney estuary, Australia. Science of the Total Environment, 512–513, 177–184.

    Google Scholar 

  • Esslinger, S., Becker, R., Jung, C., Schröter-Kermani, C., Bremsera, W., & Nehls, I. (2011). Temporal trend (1988–2008) of hexabromocyclododecane enantiomers in herring gull eggs from the German coastal region. Chemosphere, 83, 161–167.

    CAS  Google Scholar 

  • Fan, Y., Chen, S. J., Li, Q. Q., Zeng, Y., Yan, X., & Mai, B. X. (2020). Uptake of halogenated organic compounds (HOCs) into peanut and corn during the whole life cycle grown in an agricultural field. Environmental Pollution, 263, 114400.

    CAS  Google Scholar 

  • Gao, C., Xia, L., Wu, C., Wong, C. S., & Guo, Y. (2019). The effects of prosperity indices and land use indicators of an urban conurbation on the occurrence of hexabromocyclododecanes and tetrabromobisphenol A in surface soil in South China. Environmental Pollution, 252, 1810–1818.

    CAS  Google Scholar 

  • Gerecke, A. C., Giger, W., Hartmann, P. C., Heeb, N. V., Kohler, H. P. E., Schmid, P. P., Zennegg, M., & Kohler, M. (2006). Anaerobic degradation of brominated flame retardants in sewage sludge. Chemosphere, 64, 311–317.

    CAS  Google Scholar 

  • Harrad, S. J., Abdallah, M. A. E., & Covaci, A. (2009). Causes of variability in concentrations and diasteromer patterns of hexabromocyclododecanes in indoor dust. Environment International, 35, 573–579.

    CAS  Google Scholar 

  • Huang, H., Wang, D., Wan, W., & Wen, B. (2017). Hexabromocyclododecanes in soils and plants from a plastic waste treatment area in North China: occurrence, diastereomerand enantiomer-specific profiles, and metabolization. Environmental Science and Pollution Research, 24, 21625–21635.

    CAS  Google Scholar 

  • Huang, M., Li, J., Xiao, Z., & Shi, Z. (2020). Tetrabromobisphenol A and hexabromocyclododecane isomers in breast milk from the general population in Beijing, China: contamination levels, temporal trends, nursing infant’s daily intake, and risk assessment. Chemosphere, 244, 125524.

    CAS  Google Scholar 

  • Hunziker, R. W., Gonsior, S., MacGregor, J. A., Desjardins, D., Ariano, J., & Friederich, U. (2004). Fate and effect of hexabromocyclododecane in the environment. Organohalogen Compounds, 66, 2300–2305.

    Google Scholar 

  • Kim, U. J., & Oh, J. E. (2014). Tetrabromobisphenol A and hexabromocyclododecane flame retardants in infant-mother paired serum samples, and their relationships with thyroid hormones and environmental factors. Environmental Pollution, 184, 193–200.

    CAS  Google Scholar 

  • Law, R. J., Bersuder, P., Barry, J., Wilford, B. H., Allchin, C. R., & Jepson, P. D. (2008). A significant downturn in levels of hexabromocyclododecane in the blubber of harbor porpoises (Phocoena phocoena) stranded or bycaught in the UK: an update to 2006. Environmental Science & Technology, 42, 9104–9109.

    CAS  Google Scholar 

  • Li, Y., Zhou, Q., Wang, Y., & Xie, X. (2011). Fate of tetrabromobisphenol A and hexabromocyclododecane brominated flame retardants in soil and uptake by plants. Chemosphere, 82, 204–209.

    CAS  Google Scholar 

  • Li, F., Jin, J., Tan, D., Wang, L., Geng, N., Cao, R., Gao, Y., & Chen, J. (2016). Hexabromocyclododecane and tetrabromobisphenol A in sediments and paddy soils from Liaohe River Basin, China: levels, distribution and mass inventory. Journal of Environmental Sciences, 48, 209–217.

    CAS  Google Scholar 

  • Lu, J. F., He, M. J., Yang, Z. H., & Wei, S. Q. (2018). Occurrence of tetrabromobisphenol a (TBBPA) and hexabromocyclododecane (HBCDD) in soil and road dust in Chongqing, western China, with emphasis on diastereoisomer profiles, particle size distribution, and human exposure. Environmental Pollution, 242, 219–228.

    CAS  Google Scholar 

  • Lü, H., Ma, X. J., Huang, X. J., Lu, S., Huang, Y. H., Mo, C. H., Cai, Q. Y., & Wong, M. H. (2019). Distribution, diastereomer-specific accumulation and associated health risks of hexabromocyclododecanes (HBCDDs) in soil-vegetable system of the Pearl River Delta region, South China. Journal of Environmental Management, 248, 109321.

    Google Scholar 

  • Marvin, C. H., Tomy, G. T., Armitage, J. M., Arnot, J. A., McCarty, L., Covaci, A., & Palace, V. (2011). Hexabromocyclododecane: current understanding of chemistry, environmental fate and toxicology and implications for global management. Environmental Science & Technology, 45, 8613–8623.

    CAS  Google Scholar 

  • MEP (Ministry of Environmental Protection of China). (2016). The prohibition of production and use of hexabromocyclododecane in China. http://www.gov.cn/xinwen/2016-12/29/content_5154160.htm. Accessed 5 Jun 2020.

  • Morf, L. S., Tremp, J., Gloor, R., Huber, Y., Stengele, M., & Zennegg, M. (2005). Brominated flame retardants in waste electrical and electronic equipment: substance flows in a recycling plant. Environmental Science & Technology, 39, 8691–8699.

    CAS  Google Scholar 

  • Parvizian, B. A., Zhou, C., Fernando, S., Crimmins, B. S., Hopke, P. K., & Holsen, T. M. (2020). Concentrations and long-term temporal trends of hexabromocyclododecanes (HBCDDD) in lake trout and walleye from the Great Lakes. Environmental Science & Technology, 54, 6134–6141.

    CAS  Google Scholar 

  • Ruan, Y., Lam, J. C. W., Zhang, X., & Lam, P. K. S. (2018). Temporal changes and stereoisomeric compositions of 1,2,5,6,9,10-hexabromocyclododecane and 1,2-dibromo-4-(1,2-dibromoethyl)cyclohexane in marine mammals from the South China Sea. Environmental Science & Technology, 52, 2517–2526.

    CAS  Google Scholar 

  • Ruan, Y., Zhang, K., Wu, C., Wu, R., & Lam, P. K. S. (2019). A preliminary screening of HBCDD enantiomers transported by microplastics in wastewater treatment plants. Science of the Total Environment, 674, 171–178.

    CAS  Google Scholar 

  • Rüdel, H., Müller, J., Nowak, J., Ricking, M., Klein, R., & Kotthoff, M. (2017). Hexabromocyclododecane diastereomers in fish and suspended particulate matter from selected European waters—trend monitoring and environmental quality standard compliance. Environmental Science and Pollution Research, 24, 18048–18062.

    Google Scholar 

  • Shi, Y., Xu, X., Chen, J., Liang, R., Zheng, X., Shi, Y., & Wang, Y. (2018). Antioxidant gene expression and metabolic responses of earthworms (Eisenia fetida) after exposure to various concentrations of hexabromocyclododecane. Environmental Pollution, 232, 245–251.

    CAS  Google Scholar 

  • Smythe, T. A., Loseto, L. L., Bignert, A., Rosenberg, B., Budakowski, W., Halldorson, T., Pleskach, K., & Tomy, G. T. (2018). Temporal trends of brominated and fluorinated contaminants in Canadian Arctic beluga (Delphinapterus leucas). Arctic Science, 4, 388–404.

    Google Scholar 

  • Song, S. M., Duan, Y. S., Zhang, T., Zhang, B., Zhao, Z., Bai, X. Y., Xie, L., He, Y., Ouyang, J. P., Huang, X. F., & Sun, H. W. (2019). Serum concentrations of bisphenol A and its alternatives in elderly population living around e-waste recycling facilities in China: associations with fasting blood glucose. Ecotoxicology and Environmental Safety, 169, 822–828.

    CAS  Google Scholar 

  • Song, S. M., He, Y., Zhang, T., Zhu, H. K., Huang, X. F., Bai, X. Y., Zhang, B., & Kannan, K. (2020). Profiles of parabens and their metabolites in paired maternal-fetal serum, urine and amniotic fluid and their implications for placental transfer. Ecotoxicology and Environmental Safety, 191, 110235.

    CAS  Google Scholar 

  • Stockholm Convention. (2020). All POPs listed in the Stockholm Convention. http://chm.pops.int/TheConvention/ThePOPs/AllPOPs/tabid/2509/Default.aspx. Accessed 5 Jun 2020.

  • Sun, R., Luo, X., Zheng, X., Cao, K., Peng, P., Li, Q. X., & Mai, B. (2018). Hexabromocyclododecanes (HBCDDs) in fish: evidence of recent HBCDD input into the coastal environment. Marine Pollution Bulletin, 126, 357–362.

    CAS  Google Scholar 

  • Swedish Chemicals Agency. (2008). Risk assessment-hexabromocyclododecane, final report. Swedish Chemicals Agency, Sundbyberg. https://echa.europa.eu/documents/10162/661bff17-dc0a-4475-9758-40bdd6198f82. Accessed 5 Jun 2020.

  • Tang, J., Feng, J., Lia, X., & Li, G. (2014). Levels of flame retardants HBCDD, TBBPA and TBC in surface soils from an industrialized region of East China. Environmental Science: Processes & Impacts, 16, 1015–1021.

    CAS  Google Scholar 

  • Tomko, G., & McDonald, K. M. (2013). Environmental fate of hexabromocyclododecane from a new Canadian electronic recycling facility. Journal of Environmental Management, 114, 324–327.

    CAS  Google Scholar 

  • Tue, N. M., Takahashi, S., Suzuki, G., Isobe, T., Viet, P. H., Kobara, Y., Seike, N., Zhang, G., Sudaryanto, A., & Tanabe, S. (2013). Contamination of indoor dust and air by polychlorinated biphenyls and brominated flame retardants and relevance of nondietary exposure in Vietnamese informal e-waste recycling sites. Environment International, 51, 160–167.

    Google Scholar 

  • Wang, T., Han, S., Ruan, T., Wang, Y., Feng, J., & Jiang, G. (2013). Spatial distribution and inter-year variation of hexabromocyclododecane (HBCDD) and tris-(2,3-dibromopropyl) isocyanurate (TBC) in farm soils at a peri-urban region. Chemosphere, 90, 182–187.

    CAS  Google Scholar 

  • Wang, Y., Sun, H. W., Zhu, H. K., Yao, Y. M., Chen, H., Ren, C., Wu, F. C., & Kannan, K. (2018). Occurrence and distribution of organophosphate flame retardants (OPFRs) in soil and outdoor settled dust from a multi-waste recycling area in China. Science of the Total Environment, 625, 1056–1064.

    CAS  Google Scholar 

  • Wang, X., Sun, R., Chen, Y., Zhang, X., & Cui, Z. (2019). Temporal-spatial distribution and diastereoisomer pattern of hexabromocyclododecane in the vicinity of a chemical plant. Journal of Environmental Sciences, 82, 203–212.

    Google Scholar 

  • Wu, T., Wang, S., Huang, H., & Zhang, S. (2012). Diastereomer-specific uptake, translocation, and toxicity of hexabromocyclododecane diastereoisomers to maize. Journal of Agricultural and Food Chemistry, 60, 8528–8534.

    CAS  Google Scholar 

  • Wu, M. H., Han, T., Xu, G., Zang, C., Li, Y. J., Sun, R., Xu, B. T., Sun, Y., Chen, F. F., & Tang, L. (2016b). Occurrence of hexabromocyclododecane in soil and road dust from mixed-land-use areas of Shanghai, China, and its implications for human exposure. Science of the Total Environment, 559, 282–290.

    CAS  Google Scholar 

  • Wu, T., Huang, H., & Zhang, S. (2016a). Accumulation and phytotoxicity of technical hexabromocyclododecane in maize. Journal of Environmental Sciences, 42, 97–104.

    Google Scholar 

  • Yi, S., Liu, J. G., Jin, J., & Zhu, J. (2016). Assessment of the occupational and environmental risks of hexabromocyclododecane (HBCDD) in China. Chemosphere, 150, 4431–4437.

    Google Scholar 

  • Zhang, Y., Ruan, Y., Sun, H., Zhao, L., & Gan, Z. (2013). Hexabromocyclododecanes in surface sediments and a sediment core from rivers and harbor in the northern Chinese city of Tianjin. Chemosphere, 90, 1610–1616.

    CAS  Google Scholar 

  • Zhang, Y., Li, Q., Lu, Y., Jones, K., & Sweetman, A. J. (2016). Hexabromocyclododecanes (HBCDDDs) in surface soils from coastal cities in North China: correlation between diastereoisomer profiles and industrial activities. Chemosphere, 148, 504–510.

    CAS  Google Scholar 

  • Zhang, Y., Lu, Y., Wang, P., Li, Q., Zhang, M., & Johnson, A. C. (2018). Transport of Hexabromocyclododecane (HBCDD) into the soil, water and sediment from a large producer in China. Science of the Total Environment, 610–611, 94–100.

    Google Scholar 

  • Zhang, B., He, Y., Zhu, H. K., Huang, X. F., Bai, X. Y., Kannan, K., & Zhang, T. (2020). Concentrations of bisphenol A and its alternatives in paired maternal-fetal urine, serum and amniotic fluid from an e-waste dismantling area in China. Environment International, 136, 1–7.

    Google Scholar 

  • Zhu, H. K., & Kannan, K. (2018). Distribution profiles of melamine and its derivatives in indoor dust from twelve countries and the implications for human exposure. Environmental Science & Technology, 52, 12801–12808.

    CAS  Google Scholar 

  • Zhu, H., Sun, H., Zhang, Y., Xu, J., Li, B., & Zhou, Q. (2016). Uptake pathway, translocation, and isomerization of hexabromocyclododecane diastereoisomers by wheat in closed chambers. Environmental Science & Technology, 50, 2652–2659.

    CAS  Google Scholar 

  • Zhu, H., Sun, H., Yao, Y., Wang, F., Zhang, Y., & Liu, X. (2017a). Fate and adverse effects of hexabromocyclododecane diastereoisomers (HBCDDDs) in a soil-ryegrass pot system. Chemosphere, 184, 452–459.

    CAS  Google Scholar 

  • Zhu, H., Zhang, K., Sun, H., Wang, F., & Yao, Y. (2017b). Spatial and temporal distributions of hexabromocyclododecanes in the vicinity of an expanded polystyrene material manufacturing plant in Tianjin, China. Environmental Pollution, 222, 338–347.

    CAS  Google Scholar 

  • Zhu, H., Sun, H., Yao, Y., Gan, Z., Wang, Y., & Kannan, K. (2018). Legacy and alternative brominated flame retardants in outdoor dust and pine needles in mainland China: spatial trends, dust-plant partitioning and human exposure. Environmental Pollution, 243, 758–765.

    CAS  Google Scholar 

  • Zhu, H. K., Wang, Y., Sun, H., & Kannan, K. (2019). Fertilizers as a source of melamine and cyanuric acid in soils: a nationwide survey in China. Environmental Science & Technology Letters, 6, 55–61.

    CAS  Google Scholar 

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Sun analyzed and interpreted the measured data regarding the occurrence of HBCDDs in soils, and was a major contributor in writing the manuscript. Zhu performed the project supervision, writing review, and editing. All authors read and approved the final manuscript.

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Correspondence to Hongkai Zhu.

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Sun, Y., Zhu, H. Spatial and temporal distributions of hexabromocyclododecanes in surface soils of Jinan, China. Environ Monit Assess 192, 629 (2020). https://doi.org/10.1007/s10661-020-08587-6

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