Abstract

Particle/gas (P/G) partitioning can significantly affect the environmental behavior of atmospheric pollutants. In this study, we established a large-scale level IV fugacity-based multimedia model (the S-L4MF Model) based on the steady-state P/G partitioning theory. The spatial and temporal trends with the atmospheric contamination of polybrominated diphenyl ethers (PBDEs) in northeastern China under various climate conditions were simulated by the model. There is a reasonable agreement between the simulated and measured gaseous and particulate concentrations of 3 selected PBDE congeners (BDE-47, -99 and -209). For BDE-47, -99 and -209, 91.9 %, 94.8 % and 86.2 % of data points in the evaluation of the spatial trend, whereas 97.4 %, 98.2 % and 91.6 % of data points in the evaluation of the temporal trend, exhibit discrepancies between the modeled and measured data within 1 order of magnitude. The S-L4MF Model performed better than the other model with the same configuration but an equilibrium-state P/G partitioning assumption. The sensitivity and uncertainty analysis indicated that the air temperature and hexadecane-air partition coefficient were the dominant influencing factors on atmospheric concentrations. In addition, the model was successfully applied to study the inter-annual and seasonal variations of gaseous and particulate concentrations of the three PBDEs during 1971–2020 in Harbin, a northeastern Chinese city. Finally, we illustrated the potential to use the model to understand P/G partitioning behavior and the effects of snow and ice on atmospheric concentrations. In summary, the S-L4MF Model provided a powerful and effective tool for studying the environmental behavior of atmospheric organic pollutants, especially in cold regions.

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