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Title: Quantified Pore-Scale Nanoparticle Transport in Porous Media and the Implications for Colloid Filtration Theory

Authors:
; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
FOREIGN
OSTI Identifier:
1306617
Resource Type:
Journal Article
Resource Relation:
Journal Name: Langmuir; Journal Volume: 32; Journal Issue: 31
Country of Publication:
United States
Language:
ENGLISH

Citation Formats

Molnar, Ian L., Sanematsu, Paula C., Gerhard, Jason I., Willson, Clinton S., and O’Carroll, Denis M. Quantified Pore-Scale Nanoparticle Transport in Porous Media and the Implications for Colloid Filtration Theory. United States: N. p., 2016. Web. doi:10.1021/acs.langmuir.6b01233.
Molnar, Ian L., Sanematsu, Paula C., Gerhard, Jason I., Willson, Clinton S., & O’Carroll, Denis M. Quantified Pore-Scale Nanoparticle Transport in Porous Media and the Implications for Colloid Filtration Theory. United States. doi:10.1021/acs.langmuir.6b01233.
Molnar, Ian L., Sanematsu, Paula C., Gerhard, Jason I., Willson, Clinton S., and O’Carroll, Denis M. 2016. "Quantified Pore-Scale Nanoparticle Transport in Porous Media and the Implications for Colloid Filtration Theory". United States. doi:10.1021/acs.langmuir.6b01233.
@article{osti_1306617,
title = {Quantified Pore-Scale Nanoparticle Transport in Porous Media and the Implications for Colloid Filtration Theory},
author = {Molnar, Ian L. and Sanematsu, Paula C. and Gerhard, Jason I. and Willson, Clinton S. and O’Carroll, Denis M.},
abstractNote = {},
doi = {10.1021/acs.langmuir.6b01233},
journal = {Langmuir},
number = 31,
volume = 32,
place = {United States},
year = 2016,
month = 8
}
  • The recent study by Crist et al. (2004) attempted to provide pore scale insights into mechanisms responsible for controlling colloid transport in unsaturated porous media. However, because they relied on images obtained along surfaces that were open to the atmosphere, artificial evaporation resulted in 2 more critical artifacts; formation of air-water-solid (AWS) contact lines, and advection/deposition of colloids to AWS contact lines. These evaporation-related artifacts need to be addressed because they account for most of the colloid deposition at AWS contact lines reported in Crist et al. (2004)...As stated in Crist el al. (2004), ''... the front panel was removedmore » to avoid light reflections that obscured the view and, thus, exposed one side of the sand column to air''. Although a more recent paper (Crist et al., 2005) also presents results using the same methods and is therefore also affected by evaporation, we will restrict our present comments to Crist et al. (2004). Here, we show that removal of the front panel results in a sequence of three critical artifacts; (1) significant evaporation, (2) drying of thin films and formation of air-water-solid (AWS) contact lines, and (3) advection of colloids to AWS contact lines where they are deposited. As explained below, these artifacts so drastically disturbed their system that the magnitude of their observations are not likely to occur anywhere except within the most superficial few cm of soils. Before explaining these artifacts, we note that although trapping of colloids at AWS contact lines reported in Crist et al. (2004) is largely an artifact of evaporation, colloid filtration within perimeters of pendular rings is in fact a main prediction of the film straining model (Wan and Tokunaga, 1997). In that model, colloid filtration is predicted to be more efficient below a critical water saturation, when capillary connections between pendular rings become separated by adsorbed water films. In that paper we stated that ''Retardation of ideal, nonsorbing colloids can occur at two locations: trapped within individual pendular rings due to exclusion from entry into surrounding thin films and within film...'' (Wan and Tokunaga, 1997). Thus, while Crist et al. (2004) implied that the film straining model applies only to retardation of colloid transport within thin films, colloid retention within perimeters of pendular rings is a main feature of our model.« less
  • In the subsurface fluids play a critical role by transporting dissolved minerals, colloids and contaminants (sometimes over long distances), by mediating dissolution and precipitation processes and enabling chemical transformations in solution and at mineral surfaces. Although the complex geometries of fracture apertures, fracture networks and pore spaces may make it difficult to accurately predict fluid flow in saturated (single-phase) subsurface systems, well developed methods are available. The simulation of multiphase fluid flow in the subsurface is much more challenging because of the large density and/or viscosity ratios found in important applications (water/air in the vadose zone, water/oil, water/gas, gas/oil andmore » water/oil/gas in oil reservoirs, water/air/non-aqueous phase liquids (NAPL) in contaminated vadose zone systems and gas/molten rock in volcanic systems, for example). In addition, the complex behavior of fluid-fluid-solid contact lines, and its impact on dynamic contact angles, must also be taken into account, and coupled with the fluid flow. Pore network models and simple statistical physics based models such as the invasion percolation and diffusion-limited aggregation models have been used quite extensively. However, these models for multiphase fluid flow are based on simplified models for pore space geometries and simplified physics. Other methods such a lattice Boltzmann and lattice gas models, molecular dynamics, Monte Carlo methods, and particle methods such as dissipative particle dynamics and smoothed particle hydrodynamics are based more firmly on first principles, and they do not require simplified pore and/or fracture geometries. However, they are less (in some cases very much less) computationally efficient that pore network and statistical physics models. Recently a combination of continuum computation fluid dynamics, fluid-fluid interface tracking or capturing and simple models for the dependence of contact angles on fluid velocity at the contact line has been used to simulate multiphase fluid flow in fracture apertures, fracture networks and pore spaces. Fundamental conservation principles - conservation of momentum, and conservation of mass (or conservation of volume for incompressible fluids) and conservation of energy, as well as symmetries (Galilean invariance and isotropy) are central to the physics of fluids and the models used to simulate them. In molecular and mesoscale models observance of these conservation principles and symmetries at the microscopic level leads to macroscopic fluid dynamics that can be represented by the Navier Stokes equation. The remarkable fact that the flow of all simpe fluids, irrespective of their chemical nature, can be described by the Navier-Stokes equation is a result of these conservation principles and symmetries acting on the molecular level.« less
  • A level set simulation methodology developed for modeling coupled reactive transport and structure evolution has been applied to dissolution in fracture apertures and porous media. The coupled processes such as fluid flow, reactant transport and dissolution at the solid-liquid interfaces are handled simultaneously. The reaction-induced evolution of solid-liquid interfaces is captured using the level set method, with the advantage of representing the interface with sub-grid scale resolution. The coupled processes are simulated for several geometric models of fractures and porous media under various flow conditions and reaction rates. Quantitative relationships between permeability and porosity are obtained from some of themore » simulation results and compared with analytical constitutive relations (i.e., the conventional cubic law and the Carman-Kozeny law) based on simplified pore space geometries and reaction induced geometric evolutions. The drastic deviation of the simulation results from these analytical theories is explained by the development of large local concentration gradients of reactants within fracture apertures and individual pores observed in the simulation results and consequently the complex geometric evolution patterns of fracture apertures and pores due to mineral dissolution. The simulation results support the argument that traditional constitutive relations based on simplified geometries and conditions have limited applicability in predicting field scale reactive transport and that incorporation of micro-scale physics is necessary.« less