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Occurrence and Trophic Magnification of Polybrominated Environmental Pollution xxx (2016) 1e7 Contents lists available at ScienceDirect Environmental Pollution journal homepage: www.elsevier.com/locate/envpol Occurrence and trophic magnification of polybrominated diphenyl ethers (PBDEs) and their methoxylated derivatives in freshwater fish from Dianshan Lake, Shanghai, China* * Yihui Zhou a, b, Qiaofeng Chen a, Xinyu Du a, Ge Yin b, Yanling Qiu c, ,LuYed, Zhiliang Zhu a, Jianfu Zhao a a State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China b Department of Environmental Science and Analytical Chemistry, Stockholm University, SE-10691 Stockholm, Sweden c Key Laboratory of Yangtze River Water Environment (Ministry of Education), College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China d Jiading District Environmental Monitoring Station, Shanghai 201822, China article info abstract Article history: In this study, polybrominated diphenyl ethers (PBDEs) and methoxylated polybrominated diphenyl Received 31 May 2016 ethers (MeO-PBDEs) were analyzed in eleven freshwater fish species from Dianshan Lake, Shanghai, Received in revised form China. The highest concentrations of PBDEs and MeO-PBDEs were found in snakehead, with mean values 11 September 2016 À À of 38 ng g 1 lw and 4.2 ng g 1 lw, respectively. BDE-47 was the predominant congener of PBDEs, fol- Accepted 14 September 2016 lowed by BDE-154. Congener pattern variation of PBDEs was observed among different fish species, Available online xxx implying differences in biotransformation potential among fish. Yellow catfish showed highest con- centrations of BDE-99, -153 and -183, suggesting that it is more resistant to debromination than any Keywords: fi fi e fi other sh analyzed in the present study. Trophic magni cation factors were in the range of 1.35 1.81 for Yellow cat sh 0 Fish size all the PBDE congeners, but not for 2 -MeO-BDE-68. Negative relationship was observed between PBDEs Food web concentration and sample size (length and weight), indicating fish size dilution effect. Metabolism © 2016 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND Debromination license (http://creativecommons.org/licenses/by-nc-nd/4.0/). Stable isotope ratio PBDEs 1. Introduction OctaBDEs was never manufactured in China (Ni et al., 2013). China stopped PentaBDEs production in 2004, while the domestic pro- Polybrominated diphenyl ethers (PBDEs) have been produced duction of DecaBDEs increased from 26,000 metric tons (MTs) in since 1970s and widely used as an additive flame retardant in 2,000e41,500 MTs in 2005 and decreased to 20,500 MTs in 2011 (Ni textile, furniture, electronic circuitry and other materials (de Wit, et al., 2013). Due to the persistence, bioaccumulation, semi- 2002). PBDEs were first found in fish from Viskan River where volatility and adverse effects to human and wildlife, PentaBDE home to a number of textile industrial companies (Andersson and and OctaBDE have been regulated under the Stockholm Convention Blomkvist, 1981). Since then, numerous studies have been carried since 2009 (UNEP, 2015). out on the environmental exposure, (eco)-toxicology, (bio)-trans- Methoxylated polybrominated diphenyl ethers (MeO-PBDEs) formation and environmental fate of PBDEs (Covaci et al., 2003; were first identified in seals and fish in the Baltic Sea (Haglund Darnerud et al., 2001; Sjodin et al., 2003). Commercially PBDEs et al., 1997) and subsequently detected in various Baltic biota e.g. have been mainly produced in three technical products as Pen- cyanobacteria, blue mussel (Mytilus edulis), herring (Clupea hare- taBDE, OctaBDE and DecaBDE (WHO/ICPS, 1994). Among them, ngus) and guillemot (Uria aalga)(Malmvarn,€ 2007). Two of the major MeO-PBDEs, i.e. 6-MeO-BDE-47 and 20-MeO-BDE-68 have been identified as natural product in True's beaked whale (Meso- * This paper has been recommended for acceptance by Dr. Xiang-Zhou Meng. plodon mirus)(Teuten et al., 2005). Increasing concerns have been * Corresponding author. attracted to MeO-PBDEs, due to their structural similarity to PBDEs. E-mail address: [email protected] (Y. Qiu). http://dx.doi.org/10.1016/j.envpol.2016.09.043 0269-7491/© 2016 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/). Please cite this article in press as: Zhou, Y., et al., Occurrence and trophic magnification of polybrominated diphenyl ethers (PBDEs) and their methoxylated derivatives in freshwater fish from Dianshan Lake, Shanghai, China, Environmental Pollution (2016), http://dx.doi.org/10.1016/ j.envpol.2016.09.043 2 Y. Zhou et al. / Environmental Pollution xxx (2016) 1e7 Table 1 À Congener based concentrations (ng g 1 lw) of polybrominated biphenyl ethers (PBDEs) and methoxylated polybrominated biphenyl ethers (MeO-PBDEs) in freshwater fish collected from Dianshan Lake. Number Silver carp (SVC) Bighead carp (BHC) Rosy bitterling (RBL) Stone moroko (STM) Bigmouth grenadier anchovy (BGA) n ¼ 3n¼ 4 n(pool) ¼ 5 n(pool) ¼ 5 n(pool) ¼ 5 Lipid content (%) 0.57 (0.51e0.62) 0.76 (0.55e1.3) 4.7 (3.2e6.2) 3.4 (2.6e3.7) 3.5 (2.3e4.4) BDE-28 1.6a/1.3b (1.2e2.2)c 2.8/3.0 (1.4e3.7) 1.2/1.3 (0.63e1.9) 2.2/2.1 (1.8e2.7) 1.3/1.2 (1.1e1.6) BDE-47 1.6/1.9 (0.69e2.2) 0.54/0.34 (ND-1.5) 7.3/7.0 (4.5e10) 12/11 (8.2e14) 8.2/8.1 (7.1e9.4) BDE-99 NDd 0.062/ND (ND-0.25) 0.11/0.062 (ND-0.30) 0.11/0.11 (ND-0.20) 0.21/0.22 (ND-0.52) BDE-100 0.15/ND (ND-0.45) 0.12/0.052 (<LOQ-0.36) 0.069/0.047 (ND-0.21) 0.19/0.20 (0.11e0.32) 1.3/1.8 (ND-2.5) BDE-153 0.46/0.45 (0.43e0.49) 0.25/0.23 (0.092e0.46) 1.3/1.1 (0.61e1.8) 0.98/0.99 (0.39e1.6) 0.74/0.74 (0.63e0.81) BDE-154 1.2/0.56 (0.30e2.7) 0.26/0.098 (ND-0.82) 2.6/2.5 (1.2e3.8) 4.9/5.2 (3.3e6.2) 4.8/4.6 (3.9e6.4) PBDE-183 0.10/0.15 (ND-0.16) 0.17/ND (ND-0.67) 0.19/0.11 (ND-0.43) ND ND 7PBDEs 5.0/4.3 4.2/3.7 13/12 20/20 17/17 6-MeO-BDE-47 0.53/0.65 (ND-0.94) 2.0/2.5 (ND-3.2) 0.57/0.46 (0.30e1.1) 0.51/0.54 (0.38e0.62) 1.7/1.9 (1.4e2.0) 20-MeO-BDE-68 0.99/0.29 (ND-2.7) 0.16/ND (ND-0.62) 0.43/0.38 (0.18e0.80) 0.47/0.47 (0.39e0.54) 0.78/0.89 (0.31e0.98) a Mean. b Median. c Range (min-max). d Not detected. Kim et al. (2015) suggested that MeO-PBDEs showed a greater concentrations and congener patterns of PBDEs and MeO-PBDEs in biomagnification potential than PBDEs in freshwater food web. In eleven fish species from Dianshan Lake; (2) explore the trophic addition, MeO-PBDEs might transform to hydroxylated poly- magnification of PBDEs and MeO-PBDEs in the aquatic food web of brominated diphenyl ethers (OH-PBDEs) (Wan et al., 2009), a Dianshan Lake; (3) elucidate the relationship between the con- family of chemicals having the potential to disrupt the thyroid centration of contaminants and fish size. hormone system and oxidative phosphorylation (Legradi et al., 2014; Meerts et al., 2000). 2. Materials and methods Once released into the aquatic environments, PBDEs and MeO- PBDEs can be accumulated into the primary producers and bio- 2.1. Samples and sampling magnified through the food chain into the top predator. The trophic magnification of PBDEs and MeO-PBDEs in marine food webs has Eleven wild fish species were collected from Dianshan Lake been well documented in several researches (Kobayashi et al., 2015; located in Shanghai, China, in September, 2014. The fish species Losada et al., 2009; Mizukawa et al., 2013; Shao et al., 2016), included grass carp (Ctenopharyngodon idella,GRC,n¼ 5), bighead whereas fewer studies have been focused on the trophic magnifi- carp (Aristichthys nobilis, BHC, n ¼ 4), silver carp (Hypo- cation in freshwater lakes (Yu et al., 2012). Fish play an important phthalmichthys molitrix, SVC, n ¼ 3), crucian carp (Carassius auratus, role in the aquatic system, covering a wide range of trophic level in CCC, n ¼ 11), common carp (Cyprinus carpio, CMC, n ¼ 9), snake- the food web. In particular, carnivorous fish occupy a high position head (Channa argus, SNH, n ¼ 16), predatory carp (Erythroculter in the food web and are commonly consumed by humans (Cheung ilishaeformis, PDC, n ¼ 18), yellow catfish (Pelteobagrus fulvidraco, et al., 2008). With respective to environmental monitoring, fish YCF, n ¼ 23), rosy bitterling (Rhodeus sinensis, RBL, n ¼ 100 in 5 (e.g. herring) has been selected as a good matrix, serving for early pool), stone moroko (Pseudorasbora parva, STM, n ¼ 100 in 5 pool) warning of adverse effects due to the exposure of contaminants and bigmouth grenadier anchovy (Coilia ectenes,BGA,n¼ 100 in 5 (Airaksinen et al., 2014). However, the influences of biological pa- pool). All of them are common species in the freshwater ecosystem rameters (e.g. fish size) on accumulation of PBDEs and MeO-PBDEs in this region. Whole fish were directly placed on ice and trans- have not been well understood.
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