Inhibition of Hydroxyl Radical Reaction with Aromatics by Dissolved Natural Organic Matter

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Department of Chemistry, University of New Orleans, New Orleans, Louisiana 70148
Cite this: Environ. Sci. Technol. 2000, 34, 3, 444–449
Publication Date (Web):December 31, 1999
https://doi.org/10.1021/es990457c
Copyright © 2000 American Chemical Society
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Abstract

Reaction of aromatic compounds with hydroxyl radical is inhibited by dissolved natural organic matter (NOM). The degree of inhibition is significantly greater than that expected based on a simple model in which aromatic compound molecules bound to NOM are considered to be unreactive. In this study, hydroxyl radical was produced at steady-state concentrations using Fenton chemistry (H2O2 + Fe2+ → Fe3+ + HO- + HO·). Suwannee River fulvic acid and humic acid were used as NOM. The most likely mechanism for the observed inhibition is that hydroxyl radical formation occurs in microenvironmental sites remote from the aromatic compounds. In addition to changes in kinetics, pyrene hydroxyl radical reaction also exhibited a mechanistic change in the presence of fulvic acid. The mechanism changed from a reaction that was apparently first-order in pyrene to one that was apparently second-order in pyrene, indicating that pyrene self-reaction may have become the dominant mechanism in the presence of fulvic acid. Dissolved NOM causes significant changes in the rate and mechanism of hydroxyl radical degradation of aromatic compounds. Consequently, literature rate constants measured in pure water will not be useful for predicting the degradation of pollutants in environmental systems. The kinetic and mechanistic information in this study will be useful for developing improved degradation methods involving Fenton chemistry.

 Current address:  U.S. Geological Survey, 4821 Quail Crest Place, Lawrence, KS 66049-3839.

*

 Corresponding author phone:  (504)280-6323; fax:  (504) 280-6860; e-mail:  [email protected]

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