Transport Visualization for Studying Mass Trasnfer and Solute Transport in Permeable Media

Abstract

Understanding and predicting mass transfer coupled with solute transport in permeable media is central to several energy-related programs at the US Department of Energy (e.g., CO{sub 2} sequestration, nuclear waste disposal, hydrocarbon extraction, and groundwater remediation). Mass transfer is the set of processes that control movement of a chemical between mobile (advection-dominated) domains and immobile (diffusion- or sorption-dominated) domains within a permeable medium. Consequences of mass transfer on solute transport are numerous and may include (1) increased sequestration time within geologic formations; (2) reduction in average solute transport velocity by as much as several orders of magnitude; (3) long ''tails'' in concentration histories during removal of a solute from a permeable medium; (4) poor predictions of solute behavior over long time scales; and (5) changes in reaction rates due to mass transfer influences on pore-scale mixing of solutes. Our work produced four principle contributions: (1) the first comprehensive visualization of solute transport and mass transfer in heterogeneous porous media; (2) the beginnings of a theoretical framework that encompasses both macrodispersion and mass transfer within a single set of equations; (3) experimental and analytical tools necessary for understanding mixing and aqueous reaction in heterogeneous, granular porous media; (4) a clear experimental demonstration that reactive transport is often not accurately described by a simple coupling of the convection-dispersion equation with chemical reaction equations. The work shows that solute transport in heterogeneous media can be divided into 3 regimes--macrodispersion, advective mass transfer, and diffusive mass transfer--and that these regimes can be predicted quantitatively in binary media. We successfully predicted mass transfer in each of these regimes and verified the prediction by completing quantitative visualization experiments in each of the regimes, the first such experiments that show mass transfer in porous media in great detail. Experimental and theoretical work in media with pore-scale heterogeneity showed the temporal scale-dependency of mass transfer. Extension of the work into reactive transport, where mass transfer is very important to mixing, suggests a number of promising research directions for constructing better models of reactive transport and provides the experimental tools to develop and test these models. In particular, it is important to determine how the different solute spreading mechanisms in heterogeneous conductivity fields affect the rate and spatial pattern of chemical reaction. The project was conducted collaboratively between Oregon State University, Sandia National Laboratories, and the Massachusetts Institute of Technology. While each institution is submitting a copy of this final report for administrative purposes, the report is the largely the same since the project was a joint effort. This final report will outline the results of work completed and summarize publications and presentations. Manuscripts published or in press are attached, and subsequent publications will follow once published.