Study on Water-Atmosphere Interface Distribution and Concentration Fluctuation Intensities of Polybrominated Diphenyl Ethers in Great Lake
AbstractIn 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.
Blotevogel J., Mayeno A.N., Sale T.C. and Borch T. (2011). Prediction of contaminant persistence in aqueous phase: a quantum chemical approach. Environmental Science & Technology, 45(6), 2236-2242.
Cetin B. and Odabasi M. (2005). Measurement of Henry’s law constantss of seven polybrominated diphenyl ether (PBDE) congeners as a function of temperature. Atomspheric Environment., 39(29), 5273-5280.
Cetin B., Ozer S., Sofuoglu A. and Odabasi, M. (2006). Determination of Henry’s law constantss of organochlorine pesticides in deionized and saline water as a function of temperature. Atmospheric Environment., 40(24), 4538-4546.
Chen J.W., Wang D.G., Wang S.L., Qiao X.L. and Huang L.P. (2007). Quantitative structure-property relationships for direct photolysis of polybrominated diphenyl ethers. Ecxicology and Environmental Safety., 66(3), 348-352.
Crimmins B.S., Pagano J.J., Xia X.Y., Hopke P.K., Milligan M.S. and Holsen T.M (2012). Polybrominated diphenyl ethers (PBDEs): turning the corner in Greak Lakes trout 1980-2009. Environmental Science & Technology, 46(18), 9890-9897.
Fang L., Huang J., Yu G. and Wang L.N. (2008). Photochemical degradation of six polybrominated diphenyl ether congeners under ultraviolet irradiation in hexane. Chemosphere. 71(2), 258-267.
Gramatica P. 2(007). Principles of QSAR models validation L internal and external. QSAR & Combinatorial Science., 26(5), 694-701.
Gu C.G., Ju X.H., Jiang X., Wang F., Yang S.G. and Sun, C. (2009). DFT study on the bromination pattern dependence of electronic properties and their validity in quantitative structure-activity relationships of polybrominated diphenyl ethers. SAR QSAR Environmental Research. 20(3-4), 287-307.
Hites R.A. (2004). Polybrominated diphenyl ethers in the environment and people: A meta-analysis of concentrations. Environmental Science & Technology, 38(4), 945-956.
Jiang Y.F., Wang X.T., Zhu K., Wu M.H., Sheng G.Y. and Fu J.M. (2012). Occurrence, compositional patterns, and possible sources of polybrominated diphenyl ethers in agricultural soil of Shanghai, China. Chemoshpere, 89(9), 936-943.
Kemmlein S., Herzke D. and Law R.J. (2009). Brominated flame retardants in the European chemicals policy of REACH-Regulation and determination in materials. J.Chromatogr, A, 1216(3), 320-333.
Labunska I., Harrad S., Santillo D., Johnston P. and Brigden K. (2013). Levels and distribution of polybrominated diphenyl ethers in soil, sediment and dust samples collected from various electronic waste recycling sites with Guiyu town, southern China. Environmental Science: Processes & Impacts, 15(2), 503-511.
Li Y., Jiang L., Li X.L., Hu Y. and Wen J.Y. (2013). A QICAR model for metal ion toxicity established via PLS method. Chem.Res.Chin.Univ., 29(3), 568-573.
Luckey F., Fowler B. and Litten S. (2001). Establishing baseline levels of polybrominated diphenyl ethers in Lake Ontario surface waters In: Proceedings of the second international workshop on brominated flame retardants. The Swedish chemical society.
Ma Y.N., Salamova A., Venier M. and Hites R.A. (2013). Has the phase-out of PBDEs affected their atmospheric levels? Trends of PBDEs and their replacements in the Great Lakes atmosphere. Environmental Science & Technology, 47(20), 11457-11464.
Manchester-Neesvig J.B., Valters K. and Sonzogni W.C. (2001). Comparison of Polybrominated diphenyl ethers (PBDEs) and polychlorinated biphenyls (PCBs) in Lake Michigan Salmonids. Environmental Science & Technology, 35(6), 1072-1077.
Mikula P. and Svobodova, Z. (2006). Brominated flame retardants in the environment: their sources and effects (a review). Acta Veterinaria. Brno, 75(4), 587–599.
Möller A., Xie Z.Y., Sturm R., and Ebinghaus R. (2011). Polybrominated diphenyl ethers (PBDEs) and alternative vrominated flame retardants in air and seawater of the European Arctic. Environmental Pollution., 159(6), 1577-1583.
Na S., Kim M., Paek O. and Kim Y. (2013). Dietary assessment of human exposure to PBDEs in South Korea. Chemosphere. 90(5), 1736-1741.
Niu J., Shen Z., Yang Z., Long X. and Yu G. (2006). Quantitative structure-property relationships on photodegradation of polybrominated diphenyl ethers. Chemosphere. 64(4), 658-665.
Palm I.T., Cousins D., Mackay M., Tysklind C. and Metacalfe M.A. (2002). Assessing the environmental fate of chemicals of emerging concern: a case of the polybrominated diphenyl ethers. Environmental Pollution, 117(2), 195–213.
Papa E., Kovarich S. and Gramatica P. (2009). Development, Validation and inspection of the applicability domain of QSPR models for physicochemical properties of polybrominated diphenyl ethers. QSAR & Combinational Science. 28(8), 790-796.
Papa E., Kovarich S. and Gramatica P. (2011). On the use of local and global QSPRs for the prediction of physico-chemical properties of polybrominated diphenyl ethers. Molecular Informatics, 30(2-3), 232-240.
Puzyn T., Suzuki N. and Haranczyk M., (2008). How do the partitioning properties of polyhalogenated POPs change when chlorine is replaced with bromine? Environmental Science & Technology, 42(14), 5189-5195.
Wang Z.Y., Zeng X.L. and Zhai Z.C. (2008). Prediction of supercooled liquid vapor pressures and n-octanol/air partition constants for polybrominated diphenyl ethers by means of molecular descriptors from DFT method. Science of the Total Environment, 389(2-3), 296-305.
Worrall F. and Thomsen M. (2004). Quantum vs. topological descriptors in the development of molecular models of groundwater pollution by pesticides. Chemosphere., 54(4), 585-596.
Wold S. (1978). Cross-validation estimation of the number of components in factor and principal components analysis. Technometrics, 20(4), 397-405.
Xu H.Y., Zou J.W., Yu Q.S., Wang Y.H., Zhang J.Y. and Jin H.X. (2007). QSPA/QSAR models for prediction of the physicochemical properties and biological activity of polybrominated diphenyl ethers. Chemosphere, 66(10), 1998-2010.
Yogui G.T. and Sericano J.L. (2009). Polybrominated diphenyl ether flame retardant in the US marine environment: A review. Environmental International, 35(3), 655-666.
Zhu L.Y. and Hites R.A. 2004. Temporal trends and spatial distributions of brominated flame retardants in archived fishes from the Great Lakes. Environmental Science & Technology, 38(10), 2779-2784.