Exploratory assessment of sportfish consumption and polybrominated diphenyl ether exposure in New York State anglers☆
Introduction
Polybrominated diphenyl ethers (PBDEs) have been added as flame retardants to consumer products and other materials since the 1970s. PBDEs can constitute up to 30% of the weight of foams or plastics (Hooper and She, 2003). These compounds can easily enter the environment, because they are typically bound to product matrices physically, rather than chemically (Rahman et al., 2001). Like many other persistent organic pollutants (POPs), PBDEs are lipophilic (Braekevelt et al., 2003) and bioaccumulative, with relatively high concentrations measured in fish and higher trophic level wildlife (Loganathan et al., 1995; Johnson-Restrepo et al., 2005a; Muir et al., 2006). PBDEs began to attract considerable attention from the scientific and regulatory communities, after the discovery that levels in women's breast milk in Sweden had risen exponentially between 1972 and 1997 (Meironyte et al., 1999). A growing number of studies have since reported on PBDEs in human specimens from around the world, with levels in North America generally more than an order of magnitude higher than elsewhere (Hites, 2004; Sandanger et al., 2007; Johnson-Restrepo et al., 2005b; Sjödin et al., 2008). Endocrine disruption, developmental effects, and neurotoxicity have been observed in exposed laboratory animals (Birnbaum and Staskal, 2004), prompting investigators to search for associations in human populations (Hagmar et al., 2001; Bloom et al., 2008).
In response to concerns about the more persistent PBDE congeners, production and use of two commercial mixtures, referred to as the penta- and octa-bromodiphenyl ether (penta- and octa-BDE) mixtures, have been prohibited in Europe and Japan for several years, and the sole US manufacturer voluntarily ceased production in 2004. New York State (NYS) banned the use of the penta- and octa-BDE mixtures in 2006, and other states have passed comparable legislation. The deca-BDE mixture was recently banned by the European Union's highest court, though it continues to be used in the US.
Similar to other ubiquitous and bioaccumulative POPs, PBDEs can be found in animal-based human foods (Schecter et al., 2006a). Market-basket data suggest that fish have the highest levels of PBDEs (Luksemburg et al., 2004), nearly 3 times the average level in meats and 10 times that in dairy products (Schecter et al., 2006a). Still higher PBDE levels have been reported for sportfish and other non-market-basket fish (Johnson and Olson, 2001; Hale et al., 2001; Rice et al., 2002). Levels of PBDEs reported for Great Lakes sportfish are among the highest reported thus far; some ΣPBDE levels in lake trout exceeded 200 ng/g wet weight (ww) (Zhu and Hites, 2004). Fish PBDE levels exhibit a spatial pattern across the Great Lakes similar to that for PCBs (Carlson and Swackhamer, 2006), and levels of PBDEs and PCBs can be highly correlated in individual fish (Manchester-Neesvig et al., 2001).
Although some estimates indicate that fish consumption contributes nearly half of the average daily intake of PBDEs (Gill et al., 2004), others have concluded that meat consumption, because of its higher frequency, is a greater source of exposure in the US (Schecter et al., 2006a). A more recent assessment of PBDE exposure concluded that dietary exposure was responsible for only a small fraction of the PBDE blood level in the US (Lorber, 2008). Unlike other POPs, PBDEs can have significant non-occupational exposure sources other than food, such as household dust (Jones-Otazo et al., 2005).
Despite numerous studies investigating levels of PBDEs in humans, few have found strong associations between specific exposure sources and body burden. Consumption of fatty Baltic Sea fish was highly correlated with plasma BDE-47 (Sjödin et al., 2000), as was fish/shellfish consumption in Japan with breast milk PBDEs (Ohta et al., 2002). High rates of consumption of highly contaminated fish from a Lake in Norway were associated with elevated PBDE serum levels (Thomsen et al., 2008). In contrast, a study of Swedish fishermen's wives found no associations between fish consumption and serum PBDEs (Weiss et al., 2006), nor did a study of metropolitan New York City (NYC) area anglers (Morland et al., 2005). Few biomonitoring studies have collected information related to dust PBDE exposure, but recently Wu et al. (2007) reported statistically significant associations of breast milk PBDE levels with levels in house dust, as well as with dairy and meat consumption.
Sportfish consumption has been considered a significant route of exposure to POPs for residents of the Great Lakes Basin, and studies have reported associations between Great Lakes sportfish consumption and human body burden (Fitzgerald et al., 2007). The current preliminary, cross-sectional study of a sample of 36 NYS anglers was intended to generate hypotheses regarding potential associations between consumption of sportfish and PBDE body burden.
Section snippets
Sample selection
The study sample, recruitment, and specimen collection were previously described (Bloom et al., 2006). Briefly, plasma specimens were collected between 1995 and 1997 from 38 participants sampled from a subset (n=308) of participants in the New York State Angler Cohort Study (NYSACS) (Bloom et al., 2005). The NYSACS (n=18,082) was a prospective investigation of health effects in consumers of Great Lakes sportfish, among licensed anglers residing in 16 NYS counties contiguous to Lakes Erie and
Results
High and low consumers of Lake Ontario sportfish exhibited similar plasma lipid levels, demographic characteristics, and, except for sportfish and wild waterfowl consumption, similar dietary histories (Table 1). High consumers were markedly different from low consumers with respect to sportfish consumption, reporting a median of 7–11 (maximum, 24–36) and 0 (maximum, 1–6) NYS sportfish meals, respectively, in the year prior to study participation. Sixty-eight percent of high consumers ate Lake
Discussion
High consumers of Lake Ontario sportfish, when compared with low consumers, were found to have statistically significantly higher plasma levels of BDE-47, BDE-99, BDE-100, and ΣPBDE. Maximum concentrations were higher for all congeners and ΣPBDE, and the number of concentrations >LOD were statistically significantly higher, among high consumers, for BDE-47, BDE-100, and BDE-153. The number of years consuming sportfish from Lake Ontario and the consumption of high-POP Lake Ontario sportfish in
Acknowledgments
This research was funded in part by the Centers for Disease Control and Prevention (CDC) National Center for Environmental Health (NCEH) State Biomonitoring Implementation Program Grant U59CCU22339202, the Agency for Toxic Substances and Disease Registry (ATSDR), Grant H75-ATH 298338, and the Great Lakes Protection Fund, Grant RM 791-3021. The authors are grateful to Adriana Verschoor for her thoughtful review of this manuscript, and Craig Diederich for help with retrieval of archived specimens.
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This work was completed at the Wadsworth Center as part of the New York State Biomonitoring Program (Centers for Disease Control and Prevention (CDC), National Center for Environmental Health (NCEH) Grant U59CCU22339202) in cooperation with the New York State Angler Cohort Study at University at Buffalo, the State University of New York (Agency for Toxic Substances and Disease Registry (ATSDR), Grant H75-ATH 298338, and the Great Lakes Protection Fund, Grant H75-ATH 298338). The protocol for this study was reviewed and approved by the Institutional Review Boards for Protection of Human Subjects of the New York State Department of Health and the University at Buffalo, the State University of New York (protocol #s 05-015 and SPM0711204E, respectively).