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Polycyclic Aromatic Hydrocarbon (PAH) Binding to Dissolved Humic Substances (HS): Size Exclusion Effect  

Hur, Jin (School of the Environment, Clemson University)
Publication Information
Journal of Soil and Groundwater Environment / v.9, no.3, 2004 , pp. 12-19 More about this Journal
Abstract
Binding mechanisms of polycyclic aromatic hydrocarbons (PAHs) with a purified Aldrich humic acid (PAHA) and its ultrafiltration (UF) size fractions were investigated. Organic carbon normalized binding coefficient ($K_oc$) values were estimated by both a conventional Stern-Volmer fluorescence quenching technique and a modified fluorescence quenching method. Pyrene $K_oc$ values depended on PAHA concentration as well as freely dissolved pyrene concentration. Such nonlinear sorption-type behaviors suggested the existence of specific interactions. Smaller molecular size PAH (naphthalene) exhibited higher $K_oc$ value with medium-size PAHA UF fractions whereas larger size PAH (pyrene) had higher extent of binding with larger PAHA UF fractions. The inconsistent observation for naphthalene versus pyrene was well explained by size exclusion effect, one of the previously suggested specific mechanisms for PAH binding. In general, the extent of pyrene binding increased with lower pH likely due to the neutralization of acidic functional groups in HS and the subsequent increase in hydrophobic HS region. However, pyrene $K_oc$ results with a large UF fraction (>100K Da) corroborated the existence of the size exclusion effect as demonstrated by an increase in $K_oc$ values at a certain higher pH range. The size exclusion effect appears to be effective only for the specific conditions (HS size or pH) that render HS hole st겨ctures to fit a target PAH.
Keywords
humic substances (HS); polycyclic aromatic hydrocarbons (PAHs); organic carbon normalized binding coefficient (K$_{}$ oc/); sorption; size exclusion;
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1 Brown, D.G., Knightes, C.D., and Peters, C.A., 'Risk assesment for polycyclic aromatic hydrocarbon NAPLs using component fractions', Environ. Sci. Technol., 33, pp. 4357-4363 (1999)   DOI   ScienceOn
2 McCarthy, J.F., and Zachara, J.M., 'Subsurface transport of contaminants', Environ. Sci. Technol., 23, pp. 496-502 (1989)
3 Chin, Y.P., Aiken, G.R., and Danielsen, K.M., 'Binding of pyrene to aquatic and commercial humic substances: The role of molecular weight and aromaticit', Environ. Sci. Technol., 31, pp. 1630-1635 (1997)   DOI   ScienceOn
4 Chiou, C.T., Malcolm, R.L., Brinton, T.I., and Kile, D.E., 'Water solubility enhancement of some organic pollutants and pesticides by dissolved humic and fulvic acids', Environ. Sci. Technol', 20, pp. 502-508 (1986)   DOI   ScienceOn
5 Schnitzer, M., and Khan, S.U., Humic Substances in the Environment. New York, Marcel Dekker, Inc. (1972)
6 Schlautrnan, M.A., and Morgan, J.J., 'Effect of aquatic chemistry on the binding of polycyclic aromatic hydrocarbons by dissolved humic materials', Environ. Sci. Technol., 27, pp. 961-969 (1993)   DOI   ScienceOn
7 Gauthier, T.D., Shane, E.C., Guerin, W.F., Seitz, W.R., and Grant, C.L., 'Fluorescence quenching method for determining equilibrium constants for polycyclic aromatic hydrocarbons binding to dissolved humic materials', Environ. Sci. Technol., 20, pp. 1162-1166 (1986)   DOI   ScienceOn
8 Schwarzenbach, R.P., Gschwend, P.M., and Imboden, D.M., Environmental Organic Chemistry, Wiley-Interscience, New York (1993)
9 Young, T.M., and Weber, W.J., 'A distributed reactivity model for sorption by soils and sediments. 3. Effects of diagenetic processes on sorption energetic', Environ. Sci. Technol., 29, pp. 92-97 (1995)   DOI   ScienceOn
10 Edwards, N., 'Polycyclic aromatic hydrocarbons (PAHs) in the terrestrial - A Review', J. Environ. Qual., 12, pp. 427-441 (1983)   DOI   ScienceOn
11 Wershaw, R.L., 'Model for humus'. Environ. Sci. Technol., 27, pp. 814-816 (1993)   DOI   ScienceOn
12 Landrum, P.E., Nihart, S.R., Eadie, B.J., and Gardner, W.S., 'Reverse-phase separation method for determining pollutant binding to Aldrich humic acid and dissolved organic carbon of natural water', Environ. Sci. Technol., 18, pp. 187-192 (1984)   DOI
13 Hur, J., and Schlautman, M.A., 'Using selected operational descriptors to examine the heterogeneity within a bulk humic substance', Environ. Sci. Technol., 37, pp. 880-887 (2003)   DOI   ScienceOn
14 Chiou, C.T., and Kile, D.E., 'Deviations from sorption linearity onsoils of polar and nonpolar organic compounds at low relative concentrations', Environ. Sci. Technol., 32, pp. 338-343 (1998)   DOI   ScienceOn
15 Xing, B., and Pignatello, J.J., 'Dual-mode sorption of lowpolarity compounds in glassy poly(vinyl chloride) and soil organic matter', Environ. Sci. Technol., 31, pp. 792-799 (1997)   DOI   ScienceOn
16 Malcolm, R.L., and McCarthy, P., 'Limitations in the use of commercial humic acids in water and soil research', Environ. Sci. Technol., 20, pp. 904-911 (1986)   DOI   ScienceOn
17 Choudhry, G.G., Humic Substances: Structural, Photophysical, Photochemical and Free Radical Aspects and Interactions with Environmental Chemicals, Gordon and Breach Science (1984)
18 Perminova, I.V., Grechishcheva, N.Y., and Petrosyan, V.S., 'Relationships between structure and binding affinity of humic substances: Relevance of molecular descriptors', Environ. Sci. Technol., 33, pp. 3781-3787 (1999)   DOI   ScienceOn
19 Morel, F.M.M., and Hering, J.G., Principles and Applications of Aquatic Chemistry, New York, John Wiley and Sons (1993)
20 Gauthier, T.D., Seltz, W.R., and Grant, C.L., 'Effects on structural and compositional variations of dissolved humic materials on pyrene Koc value', Environ. Sci. Technol., 21, pp. 243-248 (1987)   DOI   ScienceOn
21 Carter, C.W., and Suffet, I.H., 'Binding of DDT to dissolved humic materials', Environ. Sci. Technol., 16, pp. 735-740 (1982)   DOI   ScienceOn
22 Laor, Y., and Rebhun, M., 'Evidence for nonlinear binding of PAHs to dissolved humic acids', Environ. Sci. Technol., 36, pp. 955-961 (2002)   DOI   ScienceOn
23 Chiou, C.T., Porter, P.E., and Schmedding, D.W., 'Partition equilibria of nonionic organic compounds between soil organic matter and water', Environ. Sci. Technol., 17, pp. 227-231 (1983)   DOI   ScienceOn