Study on Water-Atmosphere Interface Distribution and Concentration Fluctuation Intensities of Polybrominated Diphenyl Ethers in Great Lake

Long Jiang, Lin Liu, Yang Li, Yu Li

Abstract


In this study, the water-atmosphere interfaces distribution and concentration fluctuation intensities of polybrominated diphenyl ethers (PBDEs) in Great Lake were analyzed. Based on the selected significant quantum descriptors, bromination pattern descriptors (NPBS) and temperature descriptors by combination of variable important for projection (VIP) and correlation analysis, 35 experimental Henry’s law constants of PBDEs (transformed as lgH, represented the water-atmosphere interfaces distribution) at different temperatures were divided into modeling set (25 samples) and testing set (10 samples) to establish the quantitative structure-parameter relationship (QSPR) model for lgH at different temperatures via the optimal subset method firstly. Then, the Henry’s law constants of other unknown PBDEs at different temperatures were predicted and the water-atmosphere interfaces distribution regularity were analyzed from views of chemical quantum descriptors and substituent pattern respectively. At last, the concentration fluctuation intensities in Great Lake were discussed based on the correlation analysis between the detected concentration data and experimental Henry’s law constants. The established optimal QSPR model has shown a good fitness and predictive ability for Henry’ law constants of PBDEs, with the R2 and R2 pred of 0.985 and 0.978 respectively. From the view of chemical quantum descriptors, the lgH of PBDEs is positive correlative with EHOMO, indicating the ability to provide electron of congener molecule has played a leading role in governing the exchange ability between water-atmosphere interface; from the view of bromination pattern, both number of relative positions and each position have great influence on the water-atmosphere interface distribution, especially N2(6) and No can decrease the release of PBDEs from water to atmosphere in Great Lake. The concentration fluctuation intensity is negative correlated with the lgH linearly, the bigger solubility of congener in Great Lake, and the stronger water-atmosphere interface exchange ability and fluctuation intensity.

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