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

Liu, Min; Starchenko, Vitalii; Anovitz, Lawrence M.; Stack, Andrew G.

doi:10.1016/j.gca.2020.04.022

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

Journal Article · Mon Apr 27 00:00:00 EDT 2020 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2020.04.022· OSTI ID:1619024

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Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: LDRD; USDOE; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: 89233218CNA000001; AC05-00OR22725

OSTI ID:: 1619024

Alternate ID(s):: OSTI ID: 1645082
OSTI ID: 1775799

Report Number(s):: LA-UR--19-23804

Journal Information:: Geochimica et Cosmochimica Acta, Journal Name: Geochimica et Cosmochimica Acta Journal Issue: C Vol. 280; ISSN 0016-7037

Publisher:: Elsevier; The Geochemical Society; The Meteoritical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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