Global occurrence of polybrominated diphenyl ethers and their hydroxylated and methoxylated structural analogues in an important animal feed (fishmeal)

Polybrominated diphenyl ethers (PBDEs) and their hydroxylated (OH) and methoxylated (MeO) structural analogues have been found widely distributed in aquatic ecosystems, and may exhibit potential adverse effects to humans due to their bioaccumulative behavior through food chain. Fishmeal is an important animal feed applied around the world and is generally of marine origin. However, the levels and sources of PBDEs in fishmeal have not been thoroughly evaluated and their structural analogues have not been reported to date. The present study collected ninety-two fishmeal samples from world main fishmeal producing area to determine 27 PBDEs, 10 MeO-PBDEs and 11 OH-PBDEs. The concentrations of Σ₂₇PBDEs, Σ₁₀MeO-PBDEs and Σ₁₁OH-PBDEs were in the ranges of 0.1–1498 (mean: 75.8), 1.14–881 (37.4) and 1.00–47.5 (8.17) ng/g lipid, respectively. PBDEs were found primarily correlated with the historically commercial production, meaning higher production of certain commercial product in a country, higher corresponding PBDE congeners in local fishmeal. A market shift from penta- and octa-formulations toward deca-formulation was observed. BDE209 was identified as a major congener in fishmeal. Both the MeO-PBDEs and the OH-PBDEs were influenced by fishmeal producing areas (p < 0.001). High MeO-PBDEs were identified in the Southeast Asian fishmeal, which might be due to the suitable environmental conditions for the generation of bromoperoxidase-contained algae in local area. The ratio of two major MeO-PBDE congeners, 6-MeO-BDE47/2′-MeO-BDE68, were generally >1 in the northern hemisphere and <1 in the southern hemisphere in the present study, which was consistent with the results obtained from previous published papers. Both MeO-PBDEs and OH-PBDEs were in accordance with the specialties of naturally produced halogenated compounds.