Internal Domains of Natural Porous Media Revealed: Critical Locations for Transport, Storage, and Chemical Reaction

Zachara, John; Brantley, Sue; Chorover, Jon; Ewing, Robert; Kerisit, Sebastien; Liu, Chongxuan; Perfect, Edmund; Rother, Gernot; Stack, Andrew G.

doi:10.1021/acs.est.5b05015

Title: Internal Domains of Natural Porous Media Revealed: Critical Locations for Transport, Storage, and Chemical Reaction

Abstract

Internal pore domains exist within rocks, lithic fragments, subsurface sediments and soil aggregates. These domains, which we term internal domains in porous media (IDPM), contain a significant fraction of their porosity as nanopores, dominate the reactive surface area of diverse porous media types, and are important locations for chemical reactivity and hydrocarbon storage. Traditionally difficult to interrogate, advances in instrumentation and imaging methods are providing new insights on the physical structures and chemical attributes of IDPM. In this review we: discuss analytical methods to characterize IDPM, evaluate what has been learned about their size distributions, connectivity, and extended structures; determine whether they exhibit unique chemical reactivity; and assess potential for their inclusion in reactive transport models. Three key findings are noteworthy. 1) A combination of methods now allows complete characterization of the porosity spectrum of natural materials and its connectivity; while imaging microscopies are providing three dimensional representations of the interconnected pore network. 2) Chemical reactivity in pores <10 nm is expected to be different from micro and macropores, yet research performed to date is inconclusive on the nature, direction, and magnitude of effect. 3) Existing continuum reactive transport models treat IDPM as a sub-grid feature with average, empirical, scale-dependentmore »« less

Authors:

Zachara, John ^[1]; Brantley, Sue ^[2]; Chorover, Jon ^[3]; Ewing, Robert ^[4]; Kerisit, Sebastien ^[1]; Liu, Chongxuan ^[1]; Perfect, Edmund ^[5]; Rother, Gernot ^[6]; Stack, Andrew G. ^[6]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Pennsylvania State Univ., University Park, PA (United States)
Univ. of Arizona, Tucson, AZ (United States)
Iowa State Univ., Ames, IA (United States)
Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Publication Date:: Fri Feb 05 00:00:00 EST 2016

Research Org.:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1279392

Alternate Identifier(s):: OSTI ID: 1254594

Report Number(s):: PNNL-SA-113657
Journal ID: ISSN 0013-936X; KC0302060; ERKCC72

Grant/Contract Number:: AC05-00OR22725; AC05-76RL01830

Resource Type:: Journal Article: Accepted Manuscript

Journal Name:: Environmental Science and Technology

Additional Journal Information:: Journal Volume: 50; Journal Issue: 6; Journal ID: ISSN 0013-936X

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 58 GEOSCIENCES; pore systems; characterization; gas shale

Citation Formats


                    Zachara, John, Brantley, Sue, Chorover, Jon, Ewing, Robert, Kerisit, Sebastien, Liu, Chongxuan, Perfect, Edmund, Rother, Gernot, and Stack, Andrew G. Internal Domains of Natural Porous Media Revealed: Critical Locations for Transport, Storage, and Chemical Reaction.  United States: N. p., 2016. 
        Web.  doi:10.1021/acs.est.5b05015.

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                    Zachara, John, Brantley, Sue, Chorover, Jon, Ewing, Robert, Kerisit, Sebastien, Liu, Chongxuan, Perfect, Edmund, Rother, Gernot, & Stack, Andrew G. Internal Domains of Natural Porous Media Revealed: Critical Locations for Transport, Storage, and Chemical Reaction.  United States.  https://doi.org/10.1021/acs.est.5b05015

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                    Zachara, John, Brantley, Sue, Chorover, Jon, Ewing, Robert, Kerisit, Sebastien, Liu, Chongxuan, Perfect, Edmund, Rother, Gernot, and Stack, Andrew G. 2016.  
        "Internal Domains of Natural Porous Media Revealed: Critical Locations for Transport, Storage, and Chemical Reaction".  United States.  https://doi.org/10.1021/acs.est.5b05015.  https://www.osti.gov/servlets/purl/1279392.

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@article{osti_1279392,

  title        = {Internal Domains of Natural Porous Media Revealed: Critical Locations for Transport, Storage, and Chemical Reaction},

  author       = {Zachara, John and Brantley, Sue and Chorover, Jon and Ewing, Robert and Kerisit, Sebastien and Liu, Chongxuan and Perfect, Edmund and Rother, Gernot and Stack, Andrew G.},

  abstractNote = {Internal pore domains exist within rocks, lithic fragments, subsurface sediments and soil aggregates. These domains, which we term internal domains in porous media (IDPM), contain a significant fraction of their porosity as nanopores, dominate the reactive surface area of diverse porous media types, and are important locations for chemical reactivity and hydrocarbon storage. Traditionally difficult to interrogate, advances in instrumentation and imaging methods are providing new insights on the physical structures and chemical attributes of IDPM. In this review we: discuss analytical methods to characterize IDPM, evaluate what has been learned about their size distributions, connectivity, and extended structures; determine whether they exhibit unique chemical reactivity; and assess potential for their inclusion in reactive transport models. Three key findings are noteworthy. 1) A combination of methods now allows complete characterization of the porosity spectrum of natural materials and its connectivity; while imaging microscopies are providing three dimensional representations of the interconnected pore network. 2) Chemical reactivity in pores <10 nm is expected to be different from micro and macropores, yet research performed to date is inconclusive on the nature, direction, and magnitude of effect. 3) Existing continuum reactive transport models treat IDPM as a sub-grid feature with average, empirical, scale-dependent parameters; and are not formulated to include detailed information on pore networks. Overall we find that IDPM are key features controlling hydrocarbon release from shales in hydrofracking systems, organic matter stabilization and recalcitrance in soil, weathering and soil formation, and long term inorganic and organic contaminant behavior in the vadose zone and groundwater. We conclude with an assessment of impactful research opportunities to advance understanding of IDPM, and to incorporate their important effects in reactive transport models for improved environmental simulation and prediction.},

  doi          = {10.1021/acs.est.5b05015},

  url          = {https://www.osti.gov/biblio/1279392},
  journal      = {Environmental Science and Technology},

  issn         = {0013-936X},

  number       = 6,

  volume       = 50,

  place        = {United States},

  year         = {Fri Feb 05 00:00:00 EST 2016},

  month        = {Fri Feb 05 00:00:00 EST 2016}

}

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Title: Internal Domains of Natural Porous Media Revealed: Critical Locations for Transport, Storage, and Chemical Reaction

Abstract

Citation Formats

Micrometer-scale physical structure and microbial composition of soil macroaggregates journal, October 2013

Interfacial energy effects and the evolution of pore size distributions during quartz precipitation in sandstone journal, June 2010

Importance of porosity and transfer of matter in the rock weathering processes: two examples in central Spain journal, March 2011

Superhydrophobic states journal, June 2003

Mixing-induced precipitation: Experimental study and multiscale numerical analysis: MIXING-INDUCED PRECIPITATION journal, June 2008

Redox Behavior of Uranium at the Nanoporous Aluminum Oxide-Water Interface: Implications for Uranium Remediation journal, June 2012

A comparative study of X-ray tomographic microscopy on shales at different synchrotron facilities: ALS, APS and SLS journal, November 2012

X-ray microtomography characterization of porosity, permeability and reactive surface changes during dissolution journal, March 2011

Chemical diffusion between a fracture and the surrounding matrix: Measurement by computed tomography and modeling: DIFFUSION MEASUREMENT USING CT journal, April 2003

Solute distribution in porous rhyolite as evaluated by sequential centrifugation journal, August 2011

Petrophysical Applications of Neutron Radiography journal, January 2001

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Intragranular Diffusion: An Important Mechanism Influencing Solute Transport in Clastic Aquifers? journal, March 1990

Relationship between mineralogy and porosity in seals relevant to geologic CO2 sequestration journal, June 2014

A robust model for pore-water chemistry of clayrock journal, November 2009

Anion Exclusion and Coupling Effects in Nonsteady Transport Through Unsaturated Soils: I. Theory journal, September 1973

Validating the Scalability of Soft X-ray Spectromicroscopy for Quantitative Soil Ecology and Biogeochemistry Research journal, January 2015

An Investigation of Strong Sodium Retention Mechanisms in Nanopore Environments Using Nuclear Magnetic Resonance Spectroscopy journal, November 2011

The effect of pore size on cementation in porous rocks journal, February 2001

High-resolution X-ray computed tomography in geosciences: A review of the current technology and applications journal, August 2013

Dielectric Profile of Interfacial Water and its Effect on Double-Layer Capacitance journal, October 2011

Long-term sorption of halogenated organic chemicals by aquifer material. 2. Intraparticle diffusion journal, July 1991

Dehydration Effect on the Pore Size, Porosity, and Fractal Parameters of Shale Rocks: Ultrasmall-Angle X-ray Scattering Study journal, October 2014

Upscaling geochemical reaction rates using pore-scale network modeling journal, September 2006

Effects of spatially heterogeneous porosity on matrix diffusion as investigated by X-ray absorption imaging journal, March 2000

Modeling diffusion and adsorption in compacted bentonite: a critical review journal, March 2003

Comparison of molecular dynamics simulations with triple layer and modified Gouy–Chapman models in a 0.1M NaCl–montmorillonite system journal, November 2009

Chemical composition mapping with nanometre resolution by soft X-ray microscopy journal, September 2014

Non-Darcy flow behavior in liquid-saturated porous media journal, December 1962

Water Infiltration and Redistribution in Soil Aggregate Packings journal, February 2009

Examination of Hydrophobic Contaminant Adsorption in Mineral Micropores with Grand Canonical Monte Carlo Simulations journal, March 2003

Using X-ray computed tomography in pore structure characterization for a Berea sandstone: Resolution effect journal, November 2012

Sorptive stabilization of organic matter by microporous goethite: sorption into small pores vs. surface complexation journal, February 2007

Evaluation of positron emission tomography as a method to visualize subsurface microbial processes journal, April 2012

Two-region linear/nonlinear sorption modeling: Batch and column experiments journal, August 1999

Where fast weathering creates thin regolith and slow weathering creates thick regolith: FAST WEATHERING - THIN REGOLITH, SLOW WEATHERING - THICK REGOLITH journal, December 2012

Diagenetic changes in macro- to nano-scale porosity in the St. Peter Sandstone: An (ultra) small angle neutron scattering and backscattered electron imaging analysis journal, February 2013

Structure and Dynamics of Water on Aqueous Barium Ion and the {001} Barite Surface journal, November 2007

Diffusive Disappearance of Immiscible-Phase Organic Liquids in Fractured Geologic Media journal, September 1994

Optimal removal of topological artefacts in microtomographic images of porous materials journal, June 2011

Recommendations for the characterization of porous solids (Technical Report) journal, January 1994

A review of non-equilibrium water flow and solute transport in soil macropores: principles, controlling factors and consequences for water quality journal, June 2007

Low pore connectivity in natural rock journal, May 2012

Organic carbon distribution, speciation, and elemental correlations within soil microaggregates: Applications of STXM and NEXAFS spectroscopy journal, November 2007

Modeling the impact of nano-pores on mineralization in sedimentary rocks: IMPACT OF NANO-PORES ON MINERALIZATION journal, April 2009

Geochemical self-organization II; the reactive-infiltration instability journal, December 1987

Molecular Dynamics Simulations of Electrolyte Solutions at the (100) Goethite Surface journal, October 2006

Water retention of repellent and subcritical repellent soils: New insights from model and experimental investigations journal, January 2010

Surface geochemistry of the clay minerals journal, March 1999

Anion exclusion during transport through the unsaturated zone journal, October 1986

Desorption kinetics of radiocesium from subsurface sediments at Hanford Site, USA journal, August 2003

Thermodynamic modeling and sensitivity analysis of porewater chemistry in compacted bentonite journal, January 2004

New Calibration Technique for X-ray Absorption Studies in Single and Multiphase Flows in Packed Bed journal, January 2004

The representative sample size in shale oil rocks and nano-scale characterization of transport properties journal, July 2015

A new approach to quantification of metamorphism using ultra-small and small angle neutron scattering journal, December 2009

Electric Double Layer at the Rutile (110) Surface. 1. Structure of Surfaces and Interfacial Water from Molecular Dynamics by Use of ab Initio Potentials journal, August 2004

Characterization of transport properties of argillaceous sediments: Application to the Callovo-Oxfordian argillite journal, January 2005

Role of the soil matrix and minerals in protecting natural organic materials against biological attack journal, July 2000

Changes in reactive surface area during limestone dissolution: An experimental and modelling study journal, July 2009

Complete Restriction of 36 Cl – Diffusion by Celestite Precipitation in Densely Compacted Illite journal, April 2015

Persistence of uranium groundwater plumes: Contrasting mechanisms at two DOE sites in the groundwater–river interaction zone journal, April 2013

Pore and throat size distributions measured from synchrotron X-ray tomographic images of Fontainebleau sandstones journal, September 2000

Deterioration of a fractured carbonate caprock exposed to CO 2 -acidified brine flow : Deterioration of a fractured carbonate caprock exposed to CO journal, August 2011

Pore space relevant for gas permeability in Opalinus clay: Statistical analysis of homogeneity, percolation, and representative volume element: PORE SPACE OF OPALINUS CLAY journal, June 2013

Quantifying Soil Structure and Preferential Flow in Intact Soil Using X-ray Computed Tomography journal, July 2008

Approximate boundaries between different flow regimes in fractured rocks journal, August 2001

Nanofluidics: what is it and what can we expect from it? journal, April 2005

Physicochemical Heterogeneity Controls on Uranium Bioreduction Rates at the Field Scale journal, December 2011

Effects of pore-size controlled solubility on reactive transport in heterogeneous rock journal, January 2007

Hydrated goethite (α-FeOOH) (100) interface structure: Ordered water and surface functional groups journal, April 2010

The effect of spatially correlated blocking-up of some bonds or nodes of a network on the percolation threshold journal, August 1991

Stabilization of organic matter in temperate soils: mechanisms and their relevance under different soil conditions - a review journal, August 2006

Neutron imaging reveals internal plant water dynamics journal, January 2013

Quantitative coal characterisation by means of microfocus X-ray computer tomography, colour image analysis and back-scattered scanning electron microscopy journal, March 2001

Nanoscale Biogeocomplexity of the Organomineral Assemblage in Soil journal, January 2006

Percolation theory and its application to groundwater hydrology journal, April 1993

Hard x-ray scanning microscopy with coherent radiation: Beyond the resolution of conventional x-ray microscopes journal, June 2012

Micrometer-scale physical structure and microbial composition of soil macroaggregates
journal, October 2013

Interfacial energy effects and the evolution of pore size distributions during quartz precipitation in sandstone
journal, June 2010

Importance of porosity and transfer of matter in the rock weathering processes: two examples in central Spain
journal, March 2011

Superhydrophobic states
journal, June 2003

Mixing-induced precipitation: Experimental study and multiscale numerical analysis: MIXING-INDUCED PRECIPITATION
journal, June 2008

Redox Behavior of Uranium at the Nanoporous Aluminum Oxide-Water Interface: Implications for Uranium Remediation
journal, June 2012

A comparative study of X-ray tomographic microscopy on shales at different synchrotron facilities: ALS, APS and SLS
journal, November 2012

X-ray microtomography characterization of porosity, permeability and reactive surface changes during dissolution
journal, March 2011

Chemical diffusion between a fracture and the surrounding matrix: Measurement by computed tomography and modeling: DIFFUSION MEASUREMENT USING CT
journal, April 2003

Solute distribution in porous rhyolite as evaluated by sequential centrifugation
journal, August 2011

Petrophysical Applications of Neutron Radiography
journal, January 2001

Magnesite dissolution rates at different spatial scales: The role of mineral spatial distribution and flow velocity
journal, May 2013

Intragranular Diffusion: An Important Mechanism Influencing Solute Transport in Clastic Aquifers?
journal, March 1990

Relationship between mineralogy and porosity in seals relevant to geologic CO2 sequestration
journal, June 2014

A robust model for pore-water chemistry of clayrock
journal, November 2009

Anion Exclusion and Coupling Effects in Nonsteady Transport Through Unsaturated Soils: I. Theory
journal, September 1973

Validating the Scalability of Soft X-ray Spectromicroscopy for Quantitative Soil Ecology and Biogeochemistry Research
journal, January 2015

An Investigation of Strong Sodium Retention Mechanisms in Nanopore Environments Using Nuclear Magnetic Resonance Spectroscopy
journal, November 2011

The effect of pore size on cementation in porous rocks
journal, February 2001

High-resolution X-ray computed tomography in geosciences: A review of the current technology and applications
journal, August 2013

Dielectric Profile of Interfacial Water and its Effect on Double-Layer Capacitance
journal, October 2011

Long-term sorption of halogenated organic chemicals by aquifer material. 2. Intraparticle diffusion
journal, July 1991

Dehydration Effect on the Pore Size, Porosity, and Fractal Parameters of Shale Rocks: Ultrasmall-Angle X-ray Scattering Study
journal, October 2014

Upscaling geochemical reaction rates using pore-scale network modeling
journal, September 2006

Effects of spatially heterogeneous porosity on matrix diffusion as investigated by X-ray absorption imaging
journal, March 2000

Modeling diffusion and adsorption in compacted bentonite: a critical review
journal, March 2003

Comparison of molecular dynamics simulations with triple layer and modified Gouy–Chapman models in a 0.1M NaCl–montmorillonite system
journal, November 2009

Chemical composition mapping with nanometre resolution by soft X-ray microscopy
journal, September 2014

Non-Darcy flow behavior in liquid-saturated porous media
journal, December 1962

Water Infiltration and Redistribution in Soil Aggregate Packings
journal, February 2009

Examination of Hydrophobic Contaminant Adsorption in Mineral Micropores with Grand Canonical Monte Carlo Simulations
journal, March 2003

Using X-ray computed tomography in pore structure characterization for a Berea sandstone: Resolution effect
journal, November 2012

Sorptive stabilization of organic matter by microporous goethite: sorption into small pores vs. surface complexation
journal, February 2007

Evaluation of positron emission tomography as a method to visualize subsurface microbial processes
journal, April 2012

Two-region linear/nonlinear sorption modeling: Batch and column experiments
journal, August 1999

Where fast weathering creates thin regolith and slow weathering creates thick regolith: FAST WEATHERING - THIN REGOLITH, SLOW WEATHERING - THICK REGOLITH
journal, December 2012

Diagenetic changes in macro- to nano-scale porosity in the St. Peter Sandstone: An (ultra) small angle neutron scattering and backscattered electron imaging analysis
journal, February 2013

Structure and Dynamics of Water on Aqueous Barium Ion and the {001} Barite Surface
journal, November 2007

Diffusive Disappearance of Immiscible-Phase Organic Liquids in Fractured Geologic Media
journal, September 1994

Optimal removal of topological artefacts in microtomographic images of porous materials
journal, June 2011

Recommendations for the characterization of porous solids (Technical Report)
journal, January 1994

A review of non-equilibrium water flow and solute transport in soil macropores: principles, controlling factors and consequences for water quality
journal, June 2007

Low pore connectivity in natural rock
journal, May 2012

Organic carbon distribution, speciation, and elemental correlations within soil microaggregates: Applications of STXM and NEXAFS spectroscopy
journal, November 2007

Modeling the impact of nano-pores on mineralization in sedimentary rocks: IMPACT OF NANO-PORES ON MINERALIZATION
journal, April 2009

Geochemical self-organization II; the reactive-infiltration instability
journal, December 1987

Molecular Dynamics Simulations of Electrolyte Solutions at the (100) Goethite Surface
journal, October 2006

Water retention of repellent and subcritical repellent soils: New insights from model and experimental investigations
journal, January 2010

Surface geochemistry of the clay minerals
journal, March 1999

Anion exclusion during transport through the unsaturated zone
journal, October 1986

Desorption kinetics of radiocesium from subsurface sediments at Hanford Site, USA
journal, August 2003

Thermodynamic modeling and sensitivity analysis of porewater chemistry in compacted bentonite
journal, January 2004

New Calibration Technique for X-ray Absorption Studies in Single and Multiphase Flows in Packed Bed
journal, January 2004

The representative sample size in shale oil rocks and nano-scale characterization of transport properties
journal, July 2015

A new approach to quantification of metamorphism using ultra-small and small angle neutron scattering
journal, December 2009

Electric Double Layer at the Rutile (110) Surface. 1. Structure of Surfaces and Interfacial Water from Molecular Dynamics by Use of ab Initio Potentials
journal, August 2004

Characterization of transport properties of argillaceous sediments: Application to the Callovo-Oxfordian argillite
journal, January 2005

Role of the soil matrix and minerals in protecting natural organic materials against biological attack
journal, July 2000

Changes in reactive surface area during limestone dissolution: An experimental and modelling study
journal, July 2009

Complete Restriction of ³⁶ Cl ^– Diffusion by Celestite Precipitation in Densely Compacted Illite
journal, April 2015

Persistence of uranium groundwater plumes: Contrasting mechanisms at two DOE sites in the groundwater–river interaction zone
journal, April 2013

Pore and throat size distributions measured from synchrotron X-ray tomographic images of Fontainebleau sandstones
journal, September 2000

Deterioration of a fractured carbonate caprock exposed to CO ₂ -acidified brine flow : Deterioration of a fractured carbonate caprock exposed to CO
journal, August 2011

Pore space relevant for gas permeability in Opalinus clay: Statistical analysis of homogeneity, percolation, and representative volume element: PORE SPACE OF OPALINUS CLAY
journal, June 2013

Quantifying Soil Structure and Preferential Flow in Intact Soil Using X-ray Computed Tomography
journal, July 2008

Approximate boundaries between different flow regimes in fractured rocks
journal, August 2001

Nanofluidics: what is it and what can we expect from it?
journal, April 2005

Physicochemical Heterogeneity Controls on Uranium Bioreduction Rates at the Field Scale
journal, December 2011

Effects of pore-size controlled solubility on reactive transport in heterogeneous rock
journal, January 2007

Hydrated goethite (α-FeOOH) (100) interface structure: Ordered water and surface functional groups
journal, April 2010

The effect of spatially correlated blocking-up of some bonds or nodes of a network on the percolation threshold
journal, August 1991

Stabilization of organic matter in temperate soils: mechanisms and their relevance under different soil conditions - a review
journal, August 2006

Neutron imaging reveals internal plant water dynamics
journal, January 2013

Quantitative coal characterisation by means of microfocus X-ray computer tomography, colour image analysis and back-scattered scanning electron microscopy
journal, March 2001

Nanoscale Biogeocomplexity of the Organomineral Assemblage in Soil
journal, January 2006

Percolation theory and its application to groundwater hydrology
journal, April 1993

Hard x-ray scanning microscopy with coherent radiation: Beyond the resolution of conventional x-ray microscopes
journal, June 2012

Permeability and pore connectivity: A new model based on network simulations
journal, January 2010

Micro- and nano-environments of C sequestration in soil: A multi-elemental STXM–NEXAFS assessment of black C and organomineral associations
journal, November 2012

Nanogeochemistry: Geochemical reactions and mass transfers in nanopores
journal, January 2003