Elsevier

Environmental Pollution

Volume 213, June 2016, Pages 468-481
Environmental Pollution

Characterizing distributions, composition profiles, sources and potential health risk of polybrominated diphenyl ethers (PBDEs) in the coastal sediments from East China Sea

https://doi.org/10.1016/j.envpol.2016.02.054Get rights and content

Highlights

  • A 90-year high-resolution deposition record of PBDEs was studied.

  • The YR influenced distribution of BDE-183 and -209 in ECS.

  • Results suggested the debromination of BDE-209 in sediments.

  • PBDEs originated from local sources, surface runoff, degradation in ECS.

  • Cancer and non-cancer risks of the exposure to PBDEs were low for three age groups.

Abstract

Sediment samples (n = 20) were collected from Yangtze River Estuary (YRE) and the adjacent East China Sea (ECS) inner shelf to explore spatial and temporal distributions, environmental fate, sources and potential health risk of polybrominated diphenyl ethers (PBDEs). Concentrations of BDE-209 and total 7 PBDEs (without BDE-209; ∑7PBDEs) ranged from 62.3 to 1758 pg g−1 and from 36.9 to 233.6 pg g−1 dry weight, respectively; both of the highest values occurred near the city of Wenzhou. Concentrations of BDE-209 and ∑7PBDEs both indicated a decreasing trend from inshore areas toward outer shelf. Significantly positive linear correlations were only observed between logBDE-183 concentrations and TOC/grain size (r2 = 0.6734 and 0.5977 for TOC and grain size, respectively) as well as BDE-209 and TOC/grain size (r2 = 0.4137 and 0.5332 for TOC and grain size, respectively) in the north of 28°N, indicating that YR had significant influence on the distribution of higher brominated congeners only in the north part. Depth profiles of PBDEs in a sediment core P01 (n = 1, m = 11) collected from YRE showed that the input of BDE-209 gradually increased from 1930 to 2010, while the levels of ∑7PBDEs peaked in 1986 and obviously decreased in recent years. Partial Least-Squares Regression (PLSR) revealed that PBDEs in the coastal ECS were mainly from direct discharge of local anthropogenic activities (80.7%), followed by surface runoff of contaminated soils (15.1%), microbial degradation after sedimentation (2.6%) and photodegradation during atmospheric transportation (1.6%). The cancer risk of human exposure to BDE-209 at the 95% confidence level was 3.09 × 10−7, 1.67 × 10−7 and 8.86 × 10−7 for children, teens and adults, respectively, significantly lower than the threshold level (10−6). Hazard index (HI) calculated for non-cancer risk was also far less than 1 for the three groups, suggesting no non-cancer risk.

Introduction

As anthropogenic chemicals, polybrominated diphenyl ethers (PBDEs) have been extensively used as flame retardants in the commercial and industrial products, such as plastics, textiles, furnishing foams, electronic equipments and building materials (Ali et al., 2015, Jiang et al., 2010). There have been three primarily PBDE commercial formulations in use, i.e., Penta- (over 70% of BDE-47 and BDE-99), Octa- (over 40% of BDE-183), and Deca- (over 98% of BDE-209) BDEs (Alaee et al., 2003). In China, the domestic production of PBDEs was up to 10 000 tons in 2000, with Deca-BDE as the dominant products (Mai et al., 2005). With the rapid development of electrical and electronic industries in recent decades, China has become one of the largest consumers of PBDE flame retardants with an estimated annual growth rate of 7% (Fink et al., 2008). PBDEs are easily released into the environment during the production, application and disposal processes, because they are added in products without chemical bonding (Rahman et al., 2001). PBDE residues have been ubiquitously detected in abiotic matrices (soils, sediments, water and air) (He et al., 2014, Liu et al., 2015, Moon et al., 2012a, Sun et al., 2015) and biotic environment (marine animals, human milk, hair, blood, and adipose tissues) (Abdallah and Harrad, 2014, Kim et al., 2005, Kucharska et al., 2015, Moon et al., 2012b, Zhu et al., 2014a). The increasing concentrations of PBDEs in these matrices have drawn much attention in research and public communities around the world.

PBDEs, similar to other environmental pollutants, such as polychlorinated biphenyls (PCBs) and dichlorodiphenyltrichloroethane (DDT), are persistent, bioaccumulative and toxic, thereby presenting potential ecological risk. PBDEs enter the marine environment via surface runoff from land, discharge from industrial and municipal wastewater and deposition from atmospheric transport. They are accumulated in marine organisms, transferred and magnified along the food chain, and eventually pose adverse effects on the health of aquatic ecosystems and human (Schuhmacher et al., 2013). In addition, these trapped PBDEs can interact with compounds in the sediments and be degraded by the resident microbes (He et al., 2006), resulting in the formation of lower PBDE congeners, which are more toxic than higher brominated congeners (European Chemical Bureau, 2002). Toxicological studies have showed that PBDEs may be associated with neural development deficits, thyroid hormone disruption and cancer for human (McDonald, 2002), and some low brominated congeners may even cause subtle developmental, immunological and endocrinological effects on children (Gascon et al., 2011, Herbstman et al., 2008, Hertz-Picciotto et al., 2011). Concerns about their toxicological effects led to the banning on the production and usage of commercial Penta- and Octa-BDEs by the Stockholm Convention in 2004 (UNEP, 2009). More recently, the European Court of Justice annulled the exemption of Deca-BDE and the use of this mixture was also prohibited in European since July 2008 (BSEF, 2009). Although mass production and applications have been banned, a substantial quantity of PBDE-containing products still remain in the market and potentially cause adverse effects on human health. Moreover, Deca-BDE is still used in many Asian countries, such as China and Korea.

In general, coastal sediments are considered as major sinks and secondary sources of terrestrially derived pollutants (Li et al., 2012, Yang et al., 2012). These pollutants can cause great detriment to marine environment and human. Thus, in terms of marine environmental monitoring, the concentrations and composition profiles of PBDEs in surface sediments can provide significant information on recent contamination, and vertical residue profiles may exhibit the historical records and trends of PBDEs.

The East China Sea (ECS), located between 26 and 31°N and 121–126°E, is one of the largest marginal seas in the western Pacific of the northern hemisphere, and it is also the main sink of the Yangtze River-derived sediments (Guo et al., 2003). Additionally, the coastal ECS is adjacent to some fast-developing urban areas (Zhejiang and Fujian provinces in China), where there are several fast-growing factories producing textiles, furniture, electric and electronic equipments. Large quantities of PBDEs are used as flame retardants during the manufacturing processes. More importantly, a booming e-waste recycling center is located at Zhejiang province, where PBDEs were extensively detected in high levels in soils, water, air, hair and blood of children (Han et al., 2010, Wang et al., 2011, Zhang et al., 2011, Zhao et al., 2008). Despite a few studies (Li et al., 2012, Liu et al., 2015) regarding PBDE levels and distributions in the surface sediments of ECS, our understanding on the quantitative analysis of PBDE sources in marine sediments is very limited in this area, and little is known about the health risk of human exposure to PBDEs through food chain accumulation. Therefore, the present study aimed to evaluate the spatial and temporal distributions, the sources of PBDEs in the coastal ECS sediments and the potential health risk to human from intake of aquatic products via food chain accumulation in ECS area. Moreover, the influence of YR on PBDE distribution in coastal sediments from the ECS was investigated in detail.

Section snippets

Sample collection

Most of the suspended particulate matters and sediments discharged from the Yangtze River (YR) are deposited in the Yangtze River Delta (YRD); 32% of them transport southward with the coastal current and are ultimately buried in the inner shelf of ECS, forming a ribbon of mud areas (Liu et al., 2007). To evaluate the pollution levels of PBDEs, the surface sediments (0–2 cm) (n = 20) and a sediment core (P01, 122°21′36″ E, 31°14′24″ N) (n = 1, m = 11) were collected using a stainless steel

Concentrations of PBDEs

Summary of the PBDE concentrations and TOC contents in the surface sediments from the coastal ECS was shown in Table 1. PBDEs were found in all sediment samples with the detection frequency ranging from 82.6 to 100%, indicating the widespread distribution of PBDEs in aquatic environment of the ECS. The concentrations of ∑7PBDEs (sum of BDE-28, 47, 99, 100, 153, 154, 183) ranged from 36.9 to 233.6 pg g−1 dry weight (d.w.), with a mean value of 128.4 pg g−1 d.w.BDE-209 was found to be much more

Conclusion

PBDEs were ubiquitous in the coastal ECS sediments, with the concentrations of BDE-209 and ∑7PBDEs ranging from 62.3 to 1758 pg g−1 and from 36.9 to 233.6 pg g−1 d.w., respectively. Compared with other marine sediments, the coastal ECS was at low to moderate PBDE level. Concentrations of BDE-209 and ∑7PBDEs both decreased gradually from inshore areas toward the outer shelf, indicating the intensive influence of anthropogenic activities. Higher brominated congeners were significantly dominated

Acknowledgment

This study was financially supported by the National Natural Science Foundation of China (Grant No. 41276067). Grain size data were provided by Dr. Xiaodong Zhang (Marine Geosciences College of the Ocean University of China) and the core sedimentation rate was provided by Prof. Liguang Sun (University of Science and Technology of China), to whom we owe our great thanks. We also wish to thank the crew members of R/V Dong Fang Hong 2 for collecting sediment samples.

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