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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 » 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.« less

Authors:
 [1];  [2];  [3];  [4];  [1];  [1];  [5];  [6];  [6]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Pennsylvania State Univ., University Park, PA (United States)
  3. Univ. of Arizona, Tucson, AZ (United States)
  4. Iowa State Univ., Ames, IA (United States)
  5. Univ. of Tennessee, Knoxville, TN (United States)
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
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:
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.
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
Zachara, John, Brantley, Sue, Chorover, Jon, Ewing, Robert, Kerisit, Sebastien, Liu, Chongxuan, Perfect, Edmund, Rother, Gernot, and Stack, Andrew G. Fri . "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.
@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},
journal = {Environmental Science and Technology},
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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Works referencing / citing this record:

Interfacial reactions of Cu( ii ) adsorption and hydrolysis driven by nano-scale confinement
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