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Title: Grain detachment and transport clogging during mineral dissolution in carbonate rocks with permeable grain boundaries

Abstract

In this paper, we explore the effect of permeable grain boundaries on carbonate rock dissolution in order to improve our understanding of grain detachment and migration during reactive flow. To do so we investigated the effects of grain size and enhanced reactivity along grain boundaries on global dissolution kinetics. Variations of permeability and porosity were calculated, and exponential relationships were observed in fractured rocks. Our model employed a reactive transport framework based on the Darcy-Brinkman equation to simulate calcite dissolution in carbonate rocks composed of microporous grains and, included fluid transport along grain boundaries. The model includes fluid flow, solute transport by advection–diffusion, heterogeneous reaction between fluid and minerals and grain detachment with subsequent grain transport in macropores. The migration of solid particles due to dissolution was based on cluster analysis and local movement, and the results show that grain detachment can lead to significant decreases in permeability due to the clogging of transport pathways. Microporous media with smaller grain sizes (fine grains in this study) showed a higher average reaction rate than those with coarser grains. In addition, as the overall rates of geochemical processes are commonly affected by the presence of texture heterogeneities such as fractures, a singlemore » fracture (macropore) introduced into a microporous matrix composed of permeable grains and grain boundaries was modelled as a large channel connecting the inlet and outlet of the simulation domain. It was found that macropore clogging by grain detachment temporary decreased permeability, lowering the long-term global reaction rates. Lastly, we observed that increases in flow rate can reduce detachment and fracture clogging by reducing local dissolution along grain boundaries.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]
+ Show Author Affiliations
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1619024
Alternate Identifier(s):
OSTI ID: 1645082; OSTI ID: 1775799
Report Number(s):
LA-UR-19-23804
Journal ID: ISSN 0016-7037
Grant/Contract Number:  
AC05-00OR22725; 89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
Geochimica et Cosmochimica Acta
Additional Journal Information:
Journal Volume: 280; Journal Issue: C; Journal ID: ISSN 0016-7037
Publisher:
Elsevier; The Geochemical Society; The Meteoritical Society
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; Pore-scale reactive transport; Mineral dissolution; Grain boundary; Grain detachment

Citation Formats

Liu, Min, Starchenko, Vitalii, Anovitz, Lawrence M., and Stack, Andrew G. Grain detachment and transport clogging during mineral dissolution in carbonate rocks with permeable grain boundaries. United States: N. p., 2020. Web. doi:10.1016/j.gca.2020.04.022.
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Liu, Min, Starchenko, Vitalii, Anovitz, Lawrence M., & Stack, Andrew G. Grain detachment and transport clogging during mineral dissolution in carbonate rocks with permeable grain boundaries. United States. https://doi.org/10.1016/j.gca.2020.04.022
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Liu, Min, Starchenko, Vitalii, Anovitz, Lawrence M., and Stack, Andrew G. Mon . "Grain detachment and transport clogging during mineral dissolution in carbonate rocks with permeable grain boundaries". United States. https://doi.org/10.1016/j.gca.2020.04.022. https://www.osti.gov/servlets/purl/1619024.
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@article{osti_1619024,
title = {Grain detachment and transport clogging during mineral dissolution in carbonate rocks with permeable grain boundaries},
author = {Liu, Min and Starchenko, Vitalii and Anovitz, Lawrence M. and Stack, Andrew G.},
abstractNote = {In this paper, we explore the effect of permeable grain boundaries on carbonate rock dissolution in order to improve our understanding of grain detachment and migration during reactive flow. To do so we investigated the effects of grain size and enhanced reactivity along grain boundaries on global dissolution kinetics. Variations of permeability and porosity were calculated, and exponential relationships were observed in fractured rocks. Our model employed a reactive transport framework based on the Darcy-Brinkman equation to simulate calcite dissolution in carbonate rocks composed of microporous grains and, included fluid transport along grain boundaries. The model includes fluid flow, solute transport by advection–diffusion, heterogeneous reaction between fluid and minerals and grain detachment with subsequent grain transport in macropores. The migration of solid particles due to dissolution was based on cluster analysis and local movement, and the results show that grain detachment can lead to significant decreases in permeability due to the clogging of transport pathways. Microporous media with smaller grain sizes (fine grains in this study) showed a higher average reaction rate than those with coarser grains. In addition, as the overall rates of geochemical processes are commonly affected by the presence of texture heterogeneities such as fractures, a single fracture (macropore) introduced into a microporous matrix composed of permeable grains and grain boundaries was modelled as a large channel connecting the inlet and outlet of the simulation domain. It was found that macropore clogging by grain detachment temporary decreased permeability, lowering the long-term global reaction rates. Lastly, we observed that increases in flow rate can reduce detachment and fracture clogging by reducing local dissolution along grain boundaries.},
doi = {10.1016/j.gca.2020.04.022},
journal = {Geochimica et Cosmochimica Acta},
number = C,
volume = 280,
place = {United States},
year = {Mon Apr 27 00:00:00 EDT 2020},
month = {Mon Apr 27 00:00:00 EDT 2020}
}
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https://doi.org/10.1016/j.gca.2020.04.022
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