Levels of Polybrominated Diphenyl Ether Flame Retardants in Sediment Cores from Western Europe

The levels of 14 brominated diphenyl ether (BDE)-congeners in sediment cores from three locations in Western Europe have been determined by GC/MS (negative chemical ionization mode). Sediments from the Drammenfjord (Norway), the western Wadden Sea (The Netherlands), and the freshwater Lake Woserin (Mecklenburg-Vorpommern, Germany) showed a time-dependent pattern in the distribution of BDEs since the beginning of the industrial production of polybrominated diphenyl ether (PBDE) formulations. Two out of three commercially available PBDE formulations could be distinguished. Starting from the beginning of the 1970s, the penta-mix formulation is clearly present, but the deca-mix formulation is only present since the late 1970s. The octa-mix formulation appeared to be still absent in these sediments, as its marker-congener, BDE183, was never detected. In the cores from the western Wadden Sea and Lake Woserin, all TOC-normalized concentrations of the penta-BDE-derived congeners were leveling off in the most recent sediment layers representing 1995 and 1997, whereas those in the Drammenfjord were still increasing in 1999. The levels of BDE209, however, decreased in the most recent layer of all three cores. In Lake Woserin, the concentrations of BDE209 were much less elevated above those of the tri- to hexa-BDEs than in the other the two areas. This might be due to the absence of a significant PBDE input from sources other than the atmosphere to this rural lake. The absence of all PBDE congeners in the older layers of the three sediment cores, as well as in several 100−150-My-old layers from an extremely organic-rich marine sediment from the Kimmeridge clay formation in Dorset (UK), indicated the absence of natural production of the BDE congeners analyzed.