Occurrences and Fates of Hydroxylated Polybrominated Diphenyl Ethers in Marine Sediments in Relation to Trophodynamics

Abstract

While occurrences and origins of hydroxylated (OH-) polybrominated diphenyl ethers (PBDEs) in organisms have been reported, the fates of these compounds in abiotic matrixes and related trophodynamics are unclear. The present study measured concentrations of nine OH-PBDEs, twelve methoxylated (MeO-) PBDEs, and eleven PBDEs in marine sediments and explored the trophodynamics of OH-PBDEs in five invertebrates, eight fish, and two species of birds from Liaodong Bay, north China. While concentrations of PBDEs were less than the limit of quantification in sediments, concentrations of ΣOH-PBDEs and ΣMeO-PBDEs were 3.2-116 pg/g dry weight (dw) and 3.8-56 pg/g dw, respectively. When the detected compounds were incubated in native marine sediments the interconversion between 6-OH-BDE47 and 6-MeO-BDE47 was observed. This result is consistent with the similar spatial distributions and significant correlation between the concentrations of these naturally occurring compounds. 6-OH-BDE47 and 2'-OH-BDE68 were detected as the two major congeners in organisms collected from Liaodong Bay, and concentrations were 0.24 ± 0.005 ng/g lw (lipid weight) and 0.088 ± 0.006 ng/g lw, respectively. Biota-sediment accumulation factors (BSAFs) for invertebrates of 6-OH-BDE47 and 2'-OH-BDE68 were 0.017-0.96 and 0.19-1.5 (except for short-necked clam: 6.3), respectively. Lipid-normalized concentrations of 6-OH-BDE47 and 2'-OH-BDE68 decreased significantly with trophic level with TMFs of 0.21 and 0.15, respectively. The fates of OH-PBDEs in sediment together with their trophodynamics in marine food webs suggested that OH-PBDEs are partitioned into sediment and undergo biodilution in the marine food web.

Major sources of MeO/OH-BDEs in the East China Sea elucidated from their records and phytoplankton biomarkers

“…3, Table SI-1), whereas many previous studies have reported higher levels of 6-MeO-BDE-47 in biotic media and sediments (e. g. Kelly et al, 2008;Zhang et al, 2012).…”

“…Similarities in down-core variations and significant correlations of the 6-OH-BDE-47/6-MeO-BDE-47 pairs can be attributed to their same origin or interconversion (Wan et al, 2010b(Wan et al, , 2009. With the use of incubated slurry spiked with individual 6-MeO-BDE47, 6-OH-BDE47, and BDE-47, Zhang et al (2012) confirmed that the MeO/OH-BDEs could be converted from their corresponding OH-or MeO-congeners via bacterial methylation and demethylation, rather than biotransformation of PBDEs. The natural relationship between these MeO/OHBDEs has also been found in red algae (Malmvärn et al, 2005(Malmvärn et al, , 2008.…”

“…Their structural analogs, including methoxylated (MeO-) and hydroxylated (OH-) PBDEs, have also been widely detected in environmental substrates, such as algae (Asplund et al, 2001;Kuniyoshi et al, 1985;Malmvärn et al, 2005Malmvärn et al, , 2008, fish (Valters et al, 2005;Zhang et al, 2010), marine animals (Fu et al, 1995;Kelly et al, 2008;Liu et al, 2012), sediments (Bradley et al, 2011;Zhang et al, 2012) and even humans (Hovander et al, 2002;Lacorte and Ikonomou, 2009;Stapleton et al, 2009;Wan et al, 2010a). Some species of MeO/OH-BDEs have shown equivalent toxic effects to PBDEs , so identifying their source has attracted increasing interest.…”

Characterization of polybrominated diphenyl ethers (PBDEs) and hydroxylated and methoxylated PBDEs in soils and plants from an e-waste area, China

“…However, ortho-substituted OH-PBDEs and MeO-PBDEs have also been detected in PBDE exposure plants and animals (Qiu et al, 2007; Wang et al, 2012;Sun et al, 2013b), and meta-and parasubstituted compounds have also been found in environmental matrices Qiu et al, 2009;Sun et al, 2013a;Zhang et al, 2012). In the present study the ortho-, meta-and para-substituted OH-PBDEs and MeO-PBDEs were all detected in the soil and plant samples with 6-OH-BDE47, 6-OH-BDE85, 2 0 -OH-BDE3, 6 0 -OH-BDE99, 3 0 -OH-BDE7, 6-MeO-BDE85 and 2 0 -MeO-BDE3 as the major congeners (Figs.…”

“…Lower brominated PBDEs which are not included in the commercial mixtures have been widely detected in the environmental matrices Gerecke et al, 2005;La Guardia et al, 2007;Stapleton et al, 2004;Van den Steen et al, 2007). OH-PBDEs and MeO-PBDEs have been found in marine organisms (algae, mussel and fish), human blood, plants and abiotic samples such as surface water, snow, rain, soils and marine sediments (Bradley et al, 2011;Malmvärn et al, 2005;Sinkkonen et al, 2004;Sun et al, 2013a;Ueno et al, 2008;Verreault et al, 2005;Zhang et al, 2012). Recent studies also detected OH-PBDEs and MeO-PBDEs in organisms and plants after in vivo PBDE exposures (Marsh et al, 2006;Qiu et al, 2007;Sun et al, 2013b;Wan et al, 2010;Wang et al, 2012).…”