Geoelectrical Measurement of Multi-Scale Mass Transfer Parameters

Abstract

Mass transfer affects contaminant transport and is thought to control the efficiency of aquifer remediation at a number of sites within the Department of Energy (DOE) complex. An improved understanding of mass transfer is critical to meeting the enormous scientific and engineering challenges currently facing DOE. Informed design of site remedies and long-term stewardship of radionuclide-contaminated sites will require new cost-effective laboratory and field techniques to measure the parameters controlling mass transfer spatially and across a range of scales. In this project, we sought to capitalize on the geophysical signatures of mass transfer. Previous numerical modeling and pilot-scale field experiments suggested that mass transfer produces a geoelectrical signature—a hysteretic relation between sampled (mobile-domain) fluid conductivity and bulk (mobile + immobile) conductivity—over a range of scales relevant to aquifer remediation. In this work, we investigated the geoelectrical signature of mass transfer during tracer transport in a series of controlled experiments to determine the operation of controlling parameters, and also investigated the use of complex-resistivity (CR) as a means of quantifying mass transfer parameters in situ without tracer experiments. In an add-on component to our grant, we additionally considered nuclear magnetic resonance (NMR) to help parse mobile from immobile porosities. Including the NMR component, our revised study objectives were to: 1. Develop and demonstrate geophysical approaches to measure mass-transfer parameters spatially and over a range of scales, including the combination of electrical resistivity monitoring, tracer tests, complex resistivity, nuclear magnetic resonance, and materials characterization; and 2. Provide mass-transfer estimates for improved understanding of contaminant fate and transport at DOE sites, such as uranium transport at the Hanford 300 Area. To achieve our objectives, we implemented a 3-part research plan involving (1) development of computer codes and techniques to estimate mass-transfer parameters from time-lapse electrical data; (2) bench-scale experiments on synthetic materials and materials from cores from the Hanford 300 Area; and (3) field demonstration experiments at the DOE’s Hanford 300 Area. In a synergistic add-on to our workplan, we analyzed data from field experiments performed at the DOE Naturita Site under a separate DOE SBR grant, on which PI Day-Lewis served as co-PI. Techniques developed for application to Hanford datasets also were applied to data from Naturita. 1. Introduction The Department of Energy (DOE) faces enormous scientific and engineering challenges associated with the remediation of legacy contamination at former nuclear weapons production facilities. Selection, design and optimization of appropriate site remedies (e.g., pump-and-treat, biostimulation, or monitored natural attenuation) requires reliable predictive models of radionuclide fate and transport; however, our current modeling capabilities are limited by an incomplete understanding of multi-scale mass transfer—its rates, scales, and the heterogeneity of controlling parameters. At many DOE sites, long “tailing” behavior, concentration rebound, and slower-than-expected cleanup are observed; these observations are all consistent with multi-scale mass transfer [Haggerty and Gorelick, 1995; Haggerty et al., 2000; 2004], which renders pump-and-treat remediation and biotransformation inefficient and slow [Haggerty and Gorelick, 1994; Harvey et al., 1994; Wilson, 1997]. Despite the importance of mass transfer, there are significant uncertainties associated with controlling parameters, and the prevalence of mass transfer remains a point of debate [e.g., Hill et al., 2006; Molz et al., 2006] for lack of experimental methods to verify and measure it in situ or independently of tracer breakthrough. There is a critical need for new field-experimental techniques to measure mass transfer in-situ and estimate multi-scale and spatially variable mass-transfer parameters. The current lack of such techniques results in large parameter uncertainty, which in turn translates into enormous prediction uncertainty and cost to DOE. In this project, we considered three hydrogeophysical approaches for providing information about mass-transfer parameters: (1) the combination of electrical-resistivity tomography (ERT) and ionic tracer experiments to explore rates of exchange and relative mobile and immobile porosities; (2) complex resistivity (CR) measurements to infer the distribution of diffusive length scales active in a porous medium; and (3) nuclear magnetic resonance (NMR) to estimate mobile and immobile porosity.