期刊
ENVIRONMENTAL SCIENCE & TECHNOLOGY
卷 38, 期 22, 页码 5825-5833出版社
AMER CHEMICAL SOC
DOI: 10.1021/es049676a
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A model was developed, using an approach based on the Ideal Adsorbed Solution Theory (IAST), to predict trichloroethylene (TCE) adsorption by granular activated carbon (GAC) preloaded with natural dissolved organic matter (DOM) isolated from three surface water sources. The IAST model was formulated for a bi-solute system in which TCE and DOM single-solute uptakes were described by the Langmuir-Freundlich and Freundlich isotherms, respectively. The effect of DOM molecular size and polarity (as measured by XAD 8 resin fractionation) on TCE uptake by preloaded GAC was assessed to identify a reactive fraction of natural water DOM for the purpose of modeling competitive adsorption. Consistent with previous work that identified low molecular weight species as the most reactive with regard to preloading effects (i.e., reducing target compound uptake), the low molecular weight components of the polar (hydrophilic) and nonpolar (hydrophobic) DOM fractions, isolated using ultrafiltration (1 kDa molecular weight cutoff membrane), exhibited significant competitive effects. Furthermore, the effects of these fractions on TCE uptake were similar; therefore, they were considered together to represent a single reactive fraction of DOM. On the basis of this finding, isotherms for the <1 kDa low molecular weight DOM fraction of the whole water were measured, and molar concentrations were computed based on an average molecular weight determined using size-exclusion chromatography. The IAST model was modified to incorporate surface area reduction due to pore blockage by DOM and to reflect the hypothesis that TCE molecules can access adsorption sites which humic molecules cannot, thus preventing competition on these sites. The model was calibrated with data for TCE uptake by carbon preloaded with the <1 kDa low molecular weight DOM fraction and was verified by predicting TCE uptake by carbon preloaded with whole natural waters for both constant GAC dose (hence constant DOM loading) and variable GAC dose (hence variable DOM loading) TCE isotherms. Preloading by DOM reduced volume in GAC pores having widths smaller than 1.25 nm (likely accessible only to TCE) to a greater extent than total pore volume, suggesting preferential blockage of micropores. Such preferential pore blockage may explain, in part, why increased DOM loading decreases the fraction of the total surface area on which no competition between TCE and DOM occurs.
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