Critical Role of the Immobile Zone in Non-Fickian Two-Phase Transport: A New Paradigm.

Using a visualization setup, we characterized the solute transport in a micromodel filled with two fluid phases using direct, real-time imaging. By processing the time series of images of solute transport (dispersion) in a two fluid-phase filled micromodel, we directly delineated the change of transport hydrodynamics as a result of fluid-phase occupancy. We found that, in the water saturation range of 0.6-0.8, the macroscopic dispersion coefficient reaches its maximum value and the coefficient was 1 order of magnitude larger than that in single fluid-phase flow in the same micromodel. The experimental results indicate that this non-monotonic, non-Fickian transport is saturation- and flow-rate-dependent. Using real-time visualization of the resident concentration (averaged concentration over a representative elementary volume of the pore network), we directly estimated the hydrodynamically stagnant (immobile) zones and the mass transfer between mobile and immobile zones. We identified (a) the nonlinear contribution of the immobile zones to the non-Fickian transport under transient transport conditions and (b) the non-monotonic fate of immobile zones with respect to saturation under single and two fluid-phase conditions in a micromodel. These two findings highlight the serious flaws in the assumptions of the conventional mobile-immobile model (MIM), which is commonly used to characterize the transport under two fluid-phase conditions.

[1]  S. Gorelick,et al.  Dispersion and advection in unsaturated porous media enhanced by anion exclusion , 1991, Nature.

[2]  R. W. Cleary,et al.  Chapter 10: Movement of Solutes in Soil: Computer-Simulated and Laboratory Results , 1979 .

[3]  M. Flury,et al.  Longitudinal and lateral dispersion in an unsaturated field soil , 1999 .

[4]  D. Feinstein,et al.  STANMOD: A Suite of Windows‐Based Programs for Evaluating Solute Transport , 2004 .

[5]  F. Leij,et al.  Hydrodynamic dispersion in an unsaturated dune sand , 2003 .

[6]  W. Jury,et al.  A laboratory study of the dispersion scale effect in column outflow experiments , 1990 .

[7]  T. Mehlhorn,et al.  Transport of Multiple Tracers in Variably Saturated Humid Region Structured Soils and Semi-arid Region Laminated Sediments , 2003 .

[8]  M. Maraqa,et al.  Effects of degree of water saturation on dispersivity and immobile water in sandy soil columns , 1997 .

[9]  J. W. Biggar,et al.  Simultaneous Transport of Chloride and Water During Infiltration , 1973 .

[10]  T.-C. Jim Yeh,et al.  The effect of water content on solute transport in unsaturated porous media , 1999 .

[11]  Martin J. Blunt,et al.  Pore‐scale modeling and continuous time random walk analysis of dispersion in porous media , 2006 .

[12]  H. Loáiciga,et al.  Solute dispersion in a variably saturated sand , 2003 .

[13]  Charles F. Harvey,et al.  When good statistical models of aquifer heterogeneity go bad: A comparison of flow, dispersion, and mass transfer in connected and multivariate Gaussian hydraulic conductivity fields , 2003 .

[14]  Shahab Ayatollahi,et al.  Laboratory Study of Alkyl Ether Sulfonates for Improved Oil Recovery in High-Salinity Carbonate Reservoirs: A Case Study , 2010 .

[15]  G. Vachaud,et al.  Solute Transfer, with Exchange between Mobile and Stagnant Water, through Unsaturated Sand1 , 1977 .

[16]  D. Russo Stochastic modeling of macrodispersion for solute transport in a heterogeneous unsaturated porous formation , 1993 .

[17]  B. Berkowitz,et al.  Measurement and analysis of non-Fickian dispersion in heterogeneous porous media. , 2003, Journal of contaminant hydrology.

[18]  S. Maciejewski Numerical and experimental study of solute transport in unsaturated soils , 1993 .

[19]  Z. Fakhroueian,et al.  Wettability Alteration in Carbonates using Zirconium Oxide Nanofluids: EOR Implications , 2012 .

[20]  B. Fu,et al.  A new mobile‐immobile model for reactive solute transport with scale‐dependent dispersion , 2010 .

[21]  W. R. Gardner,et al.  Longitudinal and transverse dispersion coefficients in unsaturated plainfield sand , 1978 .

[22]  D. A. Barry,et al.  Nonequilibrium solute transport parameters and their physical significance: numerical and experimental results , 1997 .

[23]  Karsten H. Jensen,et al.  Laboratory investigations of effective flow behavior in unsaturated heterogeneous sands , 1999 .

[24]  David Russo,et al.  Stochastic analysis of flow and transport in unsaturated heterogeneous porous formation: Effects of variability in water saturation , 1998 .

[25]  S. Rodrigues,et al.  The Effect of Matrix Properties and Preferential Pathways on the Transport of Escherichia coli RS2-GFP in Single, Saturated, Variable-Aperture Fractures. , 2015, Environmental science & technology.

[26]  Peter K. Kitanidis,et al.  Experimental Investigation and Pore-Scale Modeling Interpretation of Compound-Specific Transverse Dispersion in Porous Media , 2012, Transport in Porous Media.

[27]  A. Scheidegger General Theory of Dispersion in Porous Media , 1961 .

[28]  M. Vauclin,et al.  Two‐scale modeling of solute dispersion in unsaturated double‐porosity media: Homogenization and experimental validation , 2011 .

[29]  G. Nützmann,et al.  Estimation of water saturation dependence of dispersion in unsaturated porous media: experiments and modelling analysis , 2002 .

[30]  P. J. Wierenga,et al.  Solute Transfer Through Columns of Glass Beads , 1984 .

[31]  Charles F. Harvey,et al.  What controls the apparent timescale of solute mass transfer in aquifers and soils? A comparison of experimental results , 2004 .

[32]  Roy M. Knapp,et al.  Experimental studies of in-situ microbial enhanced oil recovery , 1984 .

[33]  M. Néel,et al.  Superdispersion in homogeneous unsaturated porous media using NMR propagators. , 2013, Physical review. E, Statistical, nonlinear, and soft matter physics.

[34]  Kurt Roth,et al.  Transport of conservative chemical through an unsaturated two‐dimensional Miller‐similar medium with steady state flow , 1996 .

[35]  V. Joekar‐Niasar,et al.  Kinetics of Low-Salinity-Flooding Effect , 2015 .

[36]  Christoph Hinz,et al.  Non‐Fickian transport in homogeneous unsaturated repacked sand , 2004 .

[37]  T. Steenhuis,et al.  Quantification of colloid retention and release by straining and energy minima in variably saturated porous media. , 2013, Environmental science & technology.

[38]  J. Parker Multiphase flow and transport in porous media , 1989 .

[39]  P. J. Wierenga,et al.  Immobile water during solute transport in unsaturated sand columns , 1990 .

[40]  Y. Niibori,et al.  Hydrodynamic dispersion and mass transfer in unsaturated flow , 1999 .

[41]  M. V. Genuchten,et al.  Mass transfer studies in sorbing porous media. I. Analytical solutions , 1976 .

[42]  K. H. Coats,et al.  Dead-End Pore Volume and Dispersion in Porous Media , 1964 .

[43]  B. Ataie‐Ashtiani,et al.  Assessment of nitrate contamination in unsaturated zone of urban areas: The case study of Tehran, Iran , 2009 .

[44]  L. Devkota,et al.  Characteristics of the dispersion coefficient in miscible displacement through a glass beads medium , 1997 .

[45]  Tanguy Le Borgne,et al.  Mixing and reaction kinetics in porous media: an experimental pore scale quantification. , 2014, Environmental science & technology.

[46]  M. V. Genuchten,et al.  Review and comparison of models for describing non-equilibrium and preferential flow and transport in the vadose zone , 2003 .

[47]  William A. Jury,et al.  Field scale transport of bromide in an unsaturated soil: 2. Dispersion modeling , 1989 .

[48]  Paul T. Callaghan,et al.  Generalized approach to NMR analysis of flow and dispersion in porous media , 1997 .

[49]  F. De Smedt,et al.  Study of tracer movement through unsaturated sand , 1986 .