The Evolution of Complex DNAPL Releases: Rates of Migration and Dissolution
Grant, Gavin P
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A series of local and bench scale laboratory experiments and bench and field scale numerical simulations were conducted to develop a better understanding of the interrelationship between nonwetting phase (NWP) source zones and downgradient aqueous phase concentrations in saturated porous media contaminated by immiscible organic liquids. Specific emphasis was placed on the factors governing the rate of NWP source zone evolution and the factors governing the rate of mass transfer from the NWP to the aqueous phase. Hysteretic NWP relative permeability-saturation (krN-SW) relationships were measured at the local scale for six sands to examine the relationship between krN-SW functions and porous media type. Parameterization of the measured constitutive relationships revealed a strong correlation between mean grain diameter and the maximum value of NWP relative permeability. The measured krN-SW relationships, were validated through a bench scale experiment involving the infiltration, redistribution, and immobilisation of NWP in an initially water saturated heterogeneous porous medium. This match of simulation to experiment represents the first validation of a multiphase flow model for transient, fixed volume NWP releases. Multiphase flow simulations of the bench scale experiment were only able to reproduce the experimental observations, in both time and space, when the measured krN-SW relationships were employed. Two-dimensional field scale simulations of a fixed volume NWP release into a heterogeneous aquifer demonstrate the influence of spatially variable krN-S relationships correlated to porous media type. Both the volume of the NWP invaded porous media, and the length of time during which NWP is migrating, will be under predicted if variable (correlated) kr,N is not accounted for in the numerical model iv formulation. This under prediction is exacerbated as the mean intrinsic permeability of the release location decreases. A new, thermodynamically-based interfacial area (IFA) model was developed for use in the single-boundary layer expression of mass transfer as an alternative to existing empirical correlation expressions. The IFA model considers consistency and continuity of constitutive relationships, energy losses, effective specific interfacial area for mass transfer, and dissolution of residual NWP. A bench scale experiment involving the release and dissolution of a transient NWP source zone in heterogeneous porous media was conducted to evaluate the appropriateness of the developed IFA model when utilised to predict NWP dissolution rates. Comparison of measured downgradient dissolved phase concentrations and source zone NWP saturations in time and space with those from numerical simulations of the experiment reveal that the proposed IFA model is superior to both a local equilibrium assumption and existing empirical correlation expressions. This represents the first mass transfer model validated for the dissolution of a complex NWP source zone. Twodimensional simulations at the field scale of multiphase flow and dissolution suggest that employing existing mass transfer expressions instead of the IFA model lead to incorrect predictions of the life spans of NWP source zones, downgradient dissolved phase concentrations, and the rate of mass flux through a downgradient boundary. The practical implication of this research is that accurate numerical predictions of the evolution of a transient NWP source in porous media require consideration of krN-S relationships and NWP / aqueous phase IFA, as these factors dictate the rates of the key subsurface contaminant processes of migration and dissolution, respectively.