Abstract
We used polybrominated diphenyl ether (PBDE) data in air at 38 sites across Japan (2009-2012), which were measured by the Japan Ministry of Environment (JMOE), to elucidate the time trend and seasonality of atmospheric PBDEs. In order to address few (7% for BDE-47) to many (63% for BDE-153 and 183) non-detect data, Tobit model, also called a censored regression model was used. The model revealed that the concentrations of PBDE congeners were influenced by a combination of year, temperature, rainfall rate, and population density. Greater declines were observed for BDE-47, -99, -153 and -183 (-21, -25, -17, -23%/year, p < 0.05) than for BDE-209 (-6%/year, p = 0.065). These trends were consistent with the estimated trends of penta-, octa- and deca-BDE contained in in-use products based on domestic demand for PBDEs in Japan and product lifespan. Seasonal patterns were opposite for light congeners (BDE-47 and -99), which increased with temperature, and heavy congeners (BDE-183, and -209), which decreased with temperature. Temperature-dependent emission (evaporation) for light congeners and temperature-independent emission (abrasion) for heavy congeners, coupled with seasonality of atmospheric boundary layer height, might explain these seasonal patterns. Human population density showed a positive correlation with all PBDE congener concentrations, whereas PBDEs showed negative correlation with rainfall rate.
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