Time Trends of Atmospheric PBDEs Inferred from Archived U.K. Herbage

Aerial portions of vegetation receive the bulk of their burden of persistent organic pollutants (POPs) from the atmosphere. Vegetation can therefore be a useful indicator of the changing atmospheric burden of POPs. Samples of archived pasture, collected from Rothamsted Experimental Station in the United Kingdom between 1930 and 2004, were analyzed for a range of polybrominated diphenyl ethers (PBDEs). PBDEs could not be routinely detected in the pre-1970 samples. Thereafter, the dominant congeners BDE 28, 47, 49, 99, 100, 153, 154, and 183 were frequently detected. The general trend was (a) a rise through the 1970s; (b) a minipeak in the mid-1980s, strongly influenced by one particularly high sample for 1984; (c) values remaining high through the late 1980s/1990s; (d) an indication of a more recent decline for all congeners (except BDE-28), consistent with recent restrictions on PBDE usage in Europe. These trends were compared to recent modeled estimates of U.K. PBDE emissions. The congener profiles of technical mixtures, U.K. air, soil, and pasture were compared and shown to be broadly similar. The implications for environmental release mechanisms are discussed.