Date of Award

Summer 2004

Document Type

Dissertation

Degree Name

Doctor of Philosophy in Environmental Engineering - (Ph.D.)

Department

Civil and Environmental Engineering

First Advisor

Lisa Axe

Second Advisor

Sima Bagheri

Third Advisor

Hsin Neng Hsieh

Fourth Advisor

Demetrius T. Papageorgiou

Fifth Advisor

Trevor Tyson

Sixth Advisor

Daniel Watts

Abstract

Assessing risks associated with the release of metals into the environment and managing remedial activities requires simulation tools that depict speciation and risk with accurate mechanistic models and well-defined transport parameters. Such tools need to address the following processes: (1) aqueous speciation, (2) distribution mechanisms, (3) transport, and (4) ecological risk. The primary objective of this research is to develop a simulation tool that accounts for these processes. Speciation in the aqueous phase can be assessed with geochemical equilibrium models, such as MINEQL+. Furthermore, metal distribution can be addressed mechanistically. Studies with Pb sorption to amorphous aluminum (HAG), iron (HFO), and manganese (HMO) oxides, as well as oxide coatings, demonstrated that intraparticle diffusion is the rate-limiting mechanism in the sorption process, where best-fit surface diffusivities ranged from 10-18 to 10-15 cm2 s-1 Intraparticle surface diffusion was incorporated into the Groundwater Modeling System (GMS) to accurately simulate metal contaminant mobility where oxides are present. In the model development, the parabolic concentration layer approximation and the operator split technique were used to solve the microscopic diffusion equation coupled with macroscopic advection and dispersion. The resulting model was employed for simulating Sr90 mobility at the U.S. Department of Energy (DOE) Hanford Site. The Sr90 plume is observed to be migrating out of the 100-N area extending into other areas of the Hanford Site and beyond. Once bioavailability is understood, static or dynamic ecological risk assessments can be conducted. Employing the ERA model, a static ecological risk assessment for exposure to depleted uranium (DU) at Aberdeen and Yuma Proving Grounds (APG and YPG) revealed that a reduction in plant root weight is considered likely to occur. For most terrestrial animals at YPG, the predicted DU dose is less than that which would result in a decrease in offspring. However, for the lesser long-nosed bat, reproductive effects are expected to occur through the reduction in size and weight of offspring. At APG, based on very limited data, it is predicted that uranium uptake will not likely affect survival of terrestrial animals and aquatic species. In model validation, sampling of pocket mice, kangaroo rat, white-throated woodrat, deer, and milfoil showed that body burden concentrations fall into the distributions simulated at both sites. This static risk assessment provides a solid background for applying the dynamic approach. Overall, this research contributes to a holistic approach in developing accurate mechanistic models for simulating metal contaminant mobility and bioavailability in subsurface environments.

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