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    Characterization, Dissolution, and Enhanced Solubilization of Multicomponent Nonaqueous Phase Liquid in Porous Media

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    Author
    Carroll, Kenneth Cooper
    Issue Date
    2007
    Keywords
    multicomponent NAPL cyclodextrin remediation contaminant transport
    Advisor
    Brusseau, Mark L.
    Committee Chair
    Brusseau, Mark L.
    
    Metadata
    Show full item record
    Publisher
    The University of Arizona.
    Rights
    Copyright © is held by the author. Digital access to this material is made possible by the University Libraries, University of Arizona. Further transmission, reproduction or presentation (such as public display or performance) of protected items is prohibited except with permission of the author.
    Abstract
    Multicomponent nonaqueous phase liquids (NAPL) contaminating the subsurface can significantly inhibit remediation. One method of enhancing the rate of remediation of NAPL constituents, compared to pump-and-treat, involves source zone treatment with enhanced solubilization agents (ESAs) including cyclodextrins. Equilibrium cyclodextrin enhanced solubilization of simple 1, 2, and 3 component NAPL mixtures was examined to evaluate the applicability of Raoult's Law. The results suggest that Raoult's Law may be used to estimate equilibrium and early-time dynamic concentrations in contact with ideal NAPL mixtures, and Raoult's Law may be used to estimate cyclodextrin enhanced groundwater concentrations for ideal NAPL mixtures. Solubility enhancement of NAPL compounds was dependent on the cyclodextrin concentration and independent of NAPL composition. Column experiments and numerical modeling were used to evaluate the dissolution behavior of the NAPL mixtures in water and a cyclodextrin solution to estimate mass transfer rates. The aqueous multicomponent dissolution followed Raoult's Law, and the model-estimated lumped rate coefficients were independent of the NAPL composition. Addition of the cyclodextrin enhanced the dissolution and removal of compounds from residual NAPL due to an increase in the driving force (i.e. concentration gradient) and the mass transfer coefficient. The model results suggest that Raoult's Law is applicable for ideal NAPL mixture dissolution in water, but potential nonideality was observed and caused the model simulation to deviate from the dissolution behavior for NAPL mixture cyclodextrin experiments. The cyclodextrin dissolution experiments were less rate-limited than aqueous dissolution, and the mass transfer coefficients were quantified with the model. The results of the model suggest that NAPL mixture nonideality and intra-NAPL diffusion may also impact enhanced dissolution behavior. Additionally, the importance of NAPL mixture characterization was illustrated by evaluation of a mixture of PCE (tetrachloroethene) and diesel fuel collected from a site in Tucson, Arizona. A sample from the site was used to create mixtures with increasing PCE in the NAPL. Chemical evaluation of the complex NAPL was conducted, and physical property and phase partitioning testing was performed, which demonstrated the effect of NAPL composition on its distribution, interphase mass transfer, and potential mobilization.
    Type
    text
    Electronic Dissertation
    Degree Name
    PhD
    Degree Level
    doctoral
    Degree Program
    Hydrology
    Graduate College
    Degree Grantor
    University of Arizona
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    Dissertations

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