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

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

Journal Article · · Geochimica et Cosmochimica Acta

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.

Research Organization:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Organization:
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
Grant/Contract Number:
AC05-00OR22725; 89233218CNA000001
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, Vol. 280, Issue C; ISSN 0016-7037
Publisher:
Elsevier; The Geochemical Society; The Meteoritical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 7 works
Citation information provided by
Web of Science

References (75)

Pore-Network Modeling Dedicated to the Determination of the Petrophysical-Property Changes in the Presence of Reactive Fluid journal September 2010
A new approach to quantification of metamorphism using ultra-small and small angle neutron scattering journal December 2009
Impact of phase saturation on wormhole formation in rock matrix acidizing journal February 2018
Pore-scale imaging and modelling journal January 2013
The effect of pH, grain size, and organic ligands on biotite weathering rates journal September 2015
A calculation of the viscous force exerted by a flowing fluid on a dense swarm of particles journal December 1949
The role of pe, pH, and carbonate on the solubility of UO2 and uraninite under nominally reducing conditions journal July 1998
Porosity and pore size distribution of deeply-buried fine-grained rocks: Influence of diagenetic and metamorphic processes on shale reservoir quality and exploration journal December 2015
Pore-scale simulation of multicomponent multiphase reactive transport with dissolution and precipitation journal June 2015
Wellbore Cement Porosity Evolution in Response to Mineral Alteration during CO 2 Flooding journal December 2016
Carbonate Acidizing: Toward a Quantitative Model of the Wormholing Phenomenon journal February 1989
The oxidative dissolution mechanism of uranium dioxide. I. The effect of temperature in hydrogen carbonate medium journal October 1999
Alterations of Fractures in Carbonate Rocks by CO 2 -Acidified Brines journal August 2015
A 2.5D Reactive Transport Model for Fracture Alteration Simulation journal July 2016
Pore-scale numerical investigation of the impacts of surface roughness: Upscaling of reaction rates in rough fractures journal October 2018
Fracture Evolution in Multimineral Systems: The Role of Mineral Composition, Flow Rate, and Fracture Aperture Heterogeneity journal January 2018
Alteration and Erosion of Rock Matrix Bordering a Carbonate-Rich Shale Fracture journal July 2017
Principles of Early Development of Karst Conduits Under Natural and Man-Made Conditions Revealed by Mathematical Analysis of Numerical Models journal April 1996
Time-dependent shapes of a dissolving mineral grain: Comparisons of simulations with microfluidic experiments journal May 2020
Dissolution and deformation in fractured carbonates caused by flow of CO2-rich brine under reservoir conditions journal June 2013
Mechanisms influencing micron and nanometer-scale reaction rate patterns during dolostone dissolution journal January 2014
Effects of Coupled Chemo-Mechanical Processes on the Evolution of Pore-Size Distributions in Geological Media journal January 2015
Limestone weathering rates accelerated by micron-scale grain detachment journal September 2014
O and H diffusion in uraninite: Implications for fluid–uraninite interactions, nuclear waste disposal, and nuclear forensics journal July 2011
Three-Dimensional Pore-Scale Modeling of Fracture Evolution in Heterogeneous Carbonate Caprock Subjected to CO 2 -Enriched Brine journal March 2019
The kinetics of calcite dissolution in acetic acid solutions journal November 1998
Anti-correlated Porosity–Permeability Changes During the Dissolution of Carbonate Rocks: Experimental Evidences and Modeling journal January 2015
Carbonate acidizing: Modeling, analysis, and characterization of wormhole formation and propagation journal July 2015
Mass transfer and problems of secondary porosity creation in deeply buried hydrocarbon reservoirs journal August 1987
Influence of aperture variability on dissolutional growth of fissures in Karst Formations journal November 1998
Kinetic modeling of nitrous oxide decomposition on Fe-ZSM-5 based on parameters obtained from first-principles calculations journal July 2005
Percolation and cluster distribution. I. Cluster multiple labeling technique and critical concentration algorithm journal October 1976
Impact of grain size and rock composition on simulated rock weathering journal January 2018
Pore-scale study of dissolution-induced changes in permeability and porosity of porous media journal September 2014
Pore Scale Modeling of Reactive Transport Involved in Geologic CO2 Sequestration journal July 2009
Simulation of dissolution and precipitation in porous media: DISSOLUTION AND PRECIPITATION IN POROUS MEDIA journal October 2003
Lattice Boltzmann simulation of chemical dissolution in porous media journal March 2002
The structure of reactive grain-boundaries under stress containing confined fluids journal June 2006
Insights into rates of fracture growth and sealing from a model for quartz cementation in fractured sandstones journal October 2014
Coupled reaction-flow modeling of diagenetic changes in reservoir permeability, porosity and mineral compositions journal August 1998
Quantifying micron-scale grain detachment during weathering experiments on limestone journal January 2016
Pore-scale heterogeneous reaction rates on a dissolving limestone surface journal October 2013
High-resolution pore-scale simulation of dissolution in porous media journal April 2017
Pore-scale modelling of CO 2 storage in fractured coal journal November 2017
Numerical simulation of fluid-fluid-solid reactions in porous media journal May 2018
Impact of mineralogical heterogeneity on reactive transport modelling journal July 2017
Predictions of permeability, surface area and average dissolution rate during reactive transport in multi-mineral rocks journal November 2018
Morphology, Genesis, and Distribution of Nanometer-Scale Pores in Siliceous Mudstones of the Mississippian Barnett Shale journal November 2009
Experimental determination of porosity and permeability changes induced by injection of CO2 into carbonate rocks journal July 2009
Experimental Characterization of Porosity Structure and Transport Property Changes in Limestone Undergoing Different Dissolution Regimes journal February 2014
Dynamic reservoir-condition microtomography of reactive transport in complex carbonates: Effect of initial pore structure and initial brine pH journal May 2017
Dynamic Three-Dimensional Pore-Scale Imaging of Reaction in a Carbonate at Reservoir Conditions journal March 2015
Mineralogical and transport controls on the evolution of porous media texture using direct numerical simulation: CONTROLS ON TEXTURE EVOLUTION journal May 2017
Simulation of mineral dissolution at the pore scale with evolving fluid-solid interfaces: review of approaches and benchmark problem set journal January 2020
The dissolution kinetics of major sedimentary carbonate minerals journal July 2002
Numerical Simulation of Reactive Transport on Micro-CT Images journal July 2016
Evolution of planar fractures in limestone: The role of flow rate, mineral heterogeneity and local transport processes journal October 2018
Deciphering pore-level precipitation mechanisms journal October 2017
Pore‐scale simulation of carbonate dissolution in micro‐CT images journal February 2016
Pervasive pressure solution transfer in a quartz sand journal May 2001
Multicomponent Diffusion and Reaction in Three-Dimensional Networks:  General Kinetics journal August 1997
Mineral dissolution and wormholing from a pore-scale perspective journal August 2017
Three-dimensional simulations of fracture dissolution: FRACTURE DISSOLUTION IN 3-D journal September 2016
The Development of Wormholes in Laboratory‐Scale Fractures: Perspectives From Three‐Dimensional Simulations journal October 2018
Pore Scale Processes Associated with Subsurface CO2 Injection and Sequestration journal January 2013
Micro-Continuum Approaches for Modeling Pore-Scale Geochemical Processes journal January 2015
A network model of channel competition in fracture dissolution journal January 2006
Reactive-infiltration instabilities in rocks. Fracture dissolution journal May 2012
Reactive-infiltration instabilities in rocks. Part 2. Dissolution of a porous matrix journal December 2013
Numerical simulation of the effect of grain size on corrosion processes: Surface roughness oscillation and cluster detachment journal August 2011
A reactive transport model of neptunium migration from the potential repository at Yucca Mountain journal August 1998
Controls of Microstructure and Chemical Reactivity on the Replacement of Limestone by Fluorite Studied Using Spatially Resolved Small Angle X-ray and Neutron Scattering journal July 2019
The effect of time on the weathering of silicate minerals: why do weathering rates differ in the laboratory and field? journal December 2003
Measurement and modelling of reactive transport in geological barriers for nuclear waste containment journal January 2015
TOUGHREACT—A simulation program for non-isothermal multiphase reactive geochemical transport in variably saturated geologic media: Applications to geothermal injectivity and CO2 geological sequestration journal March 2006

Similar Records

Simulation of Coupled Processes of Flow, Transport, and Storage of CO2 in Saline Aquifers
Technical Report · Tue Sep 30 00:00:00 EDT 2014 · OSTI ID:1619024

Application of a pore-scale reactive transport model to a natural analog for reaction-induced pore alterations
Journal Article · Thu Jan 05 00:00:00 EST 2017 · Journal of Petroleum Science and Engineering · OSTI ID:1619024

Pore and Continuum Scale Study of the Effect of Subgrid Transport Heterogeneity on Redox Reaction Rates
Journal Article · Sat Aug 01 00:00:00 EDT 2015 · Geochimica et Cosmochimica Acta, 163:140-155 · OSTI ID:1619024