skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: The impact of immobile zones on the transport and retention of nanoparticles in porous media

Journal Article · · Water Resources Research
DOI:https://doi.org/10.1002/2015WR017167· OSTI ID:1234741
 [1];  [1];  [2];  [3]
  1. Univ. of Western Ontario, London, ON (Canada)
  2. Louisiana State Univ., Baton Rouge, LA (United States)
  3. Univ. of Western Ontario, London, ON (Canada); Univ. of New South Wales, Manly Vale, NSW (Australia)

Nanoparticle transport and retention within porous media is treated by conceptualizing the porous media as a series of independent collectors (e.g., Colloid Filtration Theory). This conceptualization assumes that flow phenomena near grain–grain contacts, such as immobile zones (areas of low flow), exert a negligible influence on nanoparticle transport and assumes that retention and release of particles depends only on surface chemistry. This study investigated the impact of immobile zones on nanoparticle transport and retention by employing synchrotron X–ray computed microtomography (SXCMT) to examine pore–scale silver nanoparticle distributions during transport through three sand columns: uniform iron oxide, uniform quartz, and well–graded quartz. Extended tailing was observed during the elution phase of all experiments suggesting that hydraulic retention in immobile zones, not detachment from grains, was the source of tailing. A numerical simulation of fluid flow through an SXCMT data set predicted the presence of immobile zones near grain–grain contacts. SXCMT–determined silver nanoparticle concentrations observed that significantly lower nanoparticle concentrations existed near grain–grain contacts throughout the duration of all experiments. In addition, the SXCMT–determined pore–scale concentration gradients were found to be independent of surface chemistry and grain size distribution, suggesting that immobile zones limit the diffusive transport of nanoparticles toward the collectors. Furthermore, these results suggest that the well–known overprediction of nanoparticle retention by traditional CFT may be due to ignoring the influences of grain–grain contacts and immobile zones. As such, accurate prediction of nanoparticle transport requires consideration of immobile zones and their influence on both hydraulic and surface retention.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Science Foundation ‐ Earth Sciences; Advanced Energy Consortium; Natural Sciences and Engineering Research Council of Canada (NSERC)
Grant/Contract Number:
EAR‐1128799; FG02‐94ER14466
OSTI ID:
1234741
Journal Information:
Water Resources Research, Vol. 51, Issue 11; ISSN 0043-1397
Publisher:
American Geophysical Union (AGU)Copyright Statement
Country of Publication:
United States
Language:
ENGLISH
Citation Metrics:
Cited by: 28 works
Citation information provided by
Web of Science

References (84)

Power Law Size-Distributed Heterogeneity Explains Colloid Retention on Soda Lime Glass in the Presence of Energy Barriers journal May 2014
Impact of surfactant-induced wettability alterations on DNAPL invasion in quartz and iron oxide-coated sand systems journal January 2011
DLVO interaction energy between spheroidal particles and a flat surface journal May 2000
Laboratory Assessment of the Mobility of Nanomaterials in Porous Media journal October 2004
Pore-Scale Simulations to Determine the Applied Hydrodynamic Torque and Colloid Immobilization journal February 2011
Pore-Scale Numerical and Experimental Investigation of Colloid Retention at the Secondary Energy Minimum journal February 2012
Field and Laboratory Investigations of Inactivation of Viruses (PRD1 and MS2) Attached to Iron Oxide-Coated Quartz Sand journal June 2002
Modeling microbial transport in porous media: Traditional approaches and recent developments journal June 2007
Sensitivity of the transport and retention of stabilized silver nanoparticles to physicochemical factors journal May 2013
Directing Oleate Stabilized Nanosized Silver Colloids into Organic Phases journal February 1998
Mobility of Multiwalled Carbon Nanotubes in Porous Media journal November 2009
Colloid deposition on non-ideal porous media: The influences of collector shape and roughness on the single-collector efficiency journal January 2005
Three-dimensional vortices in single pores and their effects on transport journal January 2008
Excess Colloid Retention in Porous Media as a Function of Colloid Size, Fluid Velocity, and Grain Angularity journal December 2006
Deposition and Reentrainment of Brownian Particles in Porous Media under Unfavorable Chemical Conditions:  Some Concepts and Applications journal January 2004
Coupled effects of solution chemistry and hydrodynamics on the mobility and transport of quantum dot nanomaterials in the vadose zone journal November 2010
Apparent Decreases in Colloid Deposition Rate Coefficients with Distance of Transport under Unfavorable Deposition Conditions:  A General Phenomenon journal November 2004
Kinetics of Coupled Primary- and Secondary-Minimum Deposition of Colloids under Unfavorable Chemical Conditions journal October 2007
Single-Walled Carbon Nanotubes Exhibit Limited Transport in Soil Columns journal December 2009
Upscaling colloid transport and retention under unfavorable conditions: Linking mass transfer to pore and grain topology: UPSCALING COLLOIDS journal September 2013
Direct observations of colloid retention in granular media in the presence of energy barriers, and implications for inferred mechanisms from indirect observations journal February 2010
Estimating Attachment of Nano- and Submicrometer-particles Coated with Organic Macromolecules in Porous Media: Development of an Empirical Model journal June 2010
Insights into non-Fickian solute transport in carbonates: Insights Into Non-Fickian Solute Transport in Carbonates journal May 2013
Viscous flow in multiparticle systems: Slow motion of fluids relative to beds of spherical particles journal June 1958
Quantitative nuclear magnetic resonance measurements of preasymptotic dispersion in flow through porous media journal November 2005
A Correlation for the Collector Efficiency of Brownian Particles in Clean-Bed Filtration in Sphere Packings by a Lattice-Boltzmann Method journal June 2009
Colloid transport in saturated porous media: Elimination of attachment efficiency in a new colloid transport model: Elimination of Attachment Efficiency journal May 2013
Breakdown of Colloid Filtration Theory:  Role of the Secondary Energy Minimum and Surface Charge Heterogeneities journal February 2005
Simulation of the subsurface mobility of carbon nanoparticles at the field scale journal April 2010
Modeling non-Fickian transport in geological formations as a continuous time random walk journal January 2006
New collector efficiency equation for colloid filtration in both natural and engineered flow conditions: NEW COLLECTOR EFFICIENCY EQUATION FOR COLLOID journal May 2011
Tracking Colloid Transport in Porous Media Using Discrete Flow Fields and Sensitivity of Simulated Colloid Deposition to Space Discretization journal February 2010
Dynamics of Silica Colloid Deposition and Release in Packed Beds of Aminosilane-Modified Glass Beads journal August 2000
Prediction of colloid detachment in a model porous media: hydrodynamics journal May 2000
Pore-scale study of the collector efficiency of nanoparticles in packings of nonspherical collectors journal April 2010
Hemispheres-in-Cell Geometry to Predict Colloid Deposition in Porous Media journal November 2009
Empirical correlations to estimate agglomerate size and deposition during injection of a polyelectrolyte-modified Fe0 nanoparticle at high particle concentration in saturated sand journal November 2010
Size-Dependent Hamaker Constant for Silver Nanoparticles journal September 2012
On the late-time behavior of tracer test breakthrough curves journal December 2000
Correlation Equation for Predicting Single-Collector Efficiency in Physicochemical Filtration in Saturated Porous Media journal January 2004
Deposition of Silver Nanoparticles in Geochemically Heterogeneous Porous Media: Predicting Affinity from Surface Composition Analysis journal June 2011
Modeling the coupled effects of pore space geometry and velocity on colloid transport and retention: COLLOID TRANSPORT AND RETENTION journal February 2009
Impact of nZVI stability on mobility in porous media journal February 2013
Hamaker Constants of Systems Involving Water Obtained from a Dielectric Function That Fulfills the f Sum Rule journal November 2000
Reactive transport in disordered media: Role of fluctuations in interpretation of laboratory experiments journal January 2013
Dynamics of Colloid Deposition in Porous Media: Blocking Based on Random Sequential Adsorption journal March 1995
Transport and fate of bacteria in porous media: Coupled effects of chemical conditions and pore space geometry: BACTERIA IN POROUS MEDIA journal April 2008
Investigation of the Transport and Deposition of Fullerene (C60) Nanoparticles in Quartz Sands under Varying Flow Conditions journal October 2008
Characterization of nZVI Mobility in a Field Scale Test journal February 2014
Role of Hydrodynamic Drag on Microsphere Deposition and Re-entrainment in Porous Media under Unfavorable Conditions journal June 2005
Trajectory analysis of deep-bed filtration with the sphere-in-cell porous media model journal May 1976
Tracking colloid transport in real pore structures: Comparisons with correlation equations and experimental observations: TRACKING COLLOID TRANSPORT IN REAL POROUS MEDIA journal May 2012
Resolving the Coupled Effects of Hydrodynamics and DLVO Forces on Colloid Attachment in Porous Media journal September 2007
Carboxymethyl cellulose binding to mineral substrates: Characterization by atomic force microscopy–based Force spectroscopy and quartz-crystal microbalance with dissipation monitoring journal July 2013
Transport of Cryptosporidium parvum in porous media: Long-term elution experiments and continuous time random walk filtration modeling: TRANSPORT OF C. PARVUM IN POROUS MEDIA journal October 2006
Deposition of Cryptosporidium parvum Oocysts on Natural Organic Matter Surfaces: Microscopic Evidence for Secondary Minimum Deposition in a Radial Stagnation Point Flow Cell journal February 2009
Aggregation and Deposition of Engineered Nanomaterials in Aquatic Environments: Role of Physicochemical Interactions journal September 2010
Water and waste water filtration. Concepts and applications journal November 1971
Straining and Attachment of Colloids in Physically Heterogeneous Porous Media journal May 2004
A Field-Validated Model for In Situ Transport of Polymer-Stabilized nZVI and Implications for Subsurface Injection journal June 2013
Direct microscopic observation of particle deposition in porous media: Role of the secondary energy minimum journal February 2007
Hamaker Constants of Iron Oxide Nanoparticles journal July 2011
Pore-scale simulation of intragranular diffusion: Effects of incomplete mixing on macroscopic manifestations: Pore-Scale Simulation of Intragranular Diffusion journal July 2013
Signature of Non-Fickian Solute Transport in Complex Heterogeneous Porous Media journal November 2011
Transport and straining of E. coli O157:H7 in saturated porous media : TRANSPORT AND STRAINING OF journal November 2006
In situ testing of metallic iron nanoparticle mobility and reactivity in a shallow granular aquifer journal July 2010
Release of Colloids from Primary Minimum Contact under Unfavorable Conditions by Perturbations in Ionic Strength and Flow Rate journal July 2014
Predictions of non-Fickian solute transport in different classes of porous media using direct simulation on pore-scale images journal January 2013
Deviation from the Classical Colloid Filtration Theory in the Presence of Repulsive DLVO Interactions journal December 2004
Velocity Effects on Fullerene and Oxide Nanoparticle Deposition in Porous Media journal August 2004
Origins of anomalous transport in heterogeneous media: Structural and dynamic controls journal February 2014
Role of Low Flow and Backward Flow Zones on Colloid Transport in Pore Structures Derived from Real Porous Media journal July 2010
Quantitative characterization of pore-scale disorder effects on transport in “homogeneous” granular media journal October 2004
Microscale simulation of particle deposition in porous media journal March 2014
Impact of Porous Media Grain Size on the Transport of Multi-walled Carbon Nanotubes journal November 2011
Method for Obtaining Silver Nanoparticle Concentrations within a Porous Medium via Synchrotron X-ray Computed Microtomography journal January 2014
Key Factors Controlling the Transport of Silver Nanoparticles in Porous Media journal April 2013
Nanoscale zero valent iron and bimetallic particles for contaminated site remediation journal January 2013
Sorption of Silver Nanoparticles to Environmental and Model Surfaces journal May 2013
Colloid Transport in Geochemically Heterogeneous Porous Media:  Modeling and Measurements journal October 1996
Uniform quartz - Silver nanoparticle injection experiment dataset January 2016
Straining and Attachment of Colloids in Physically Heterogeneous Porous Media journal May 2004
Mobility of Multiwalled Carbon Nanotubes in Porous Media journal February 2010
Hemispheres-in-Cell Geometry to Predict Colloid Deposition in Porous Media journal April 2010

Cited By (3)

A binomial modeling approach for upscaling colloid transport under unfavorable conditions: Emergent prediction of extended tailing: BINOMIAL MODELING OF COLLOID TRANSPORT journal July 2017
Colloid Transport in Porous Media: A Review of Classical Mechanisms and Emerging Topics journal March 2019
Solute transport in porous media studied by lattice Boltzmann simulations at pore scale and x-ray tomography experiments journal December 2019