“…In this study, a microcontinuum reactive transport model was used to illustrate the mineral reaction front migration and test the impacts of matrix properties. The reactive transport model has been detailed in previous studies, ,− and the simulation setup for this study is described here.…”
Hydraulic fracturing of shale reservoirs resulted in
significant
opportunities for increased oil and gas production in the United States.
Rock–fluid interactions can cause mineral dissolution and precipitation
reactions that lead to permeability changes in the shale matrix, which
ultimately may affect transport pathways and hydrocarbon production.
Understanding the distribution of secondary precipitates, such as
barite and Fe(III) (hydro)oxides, and cation leaching at the rock–fluid
interface is an important step to further investigate how these geochemical
processes can change permeability and transport pathways. In this
study, thin sections of the fracture-matrix interface were made from
reacted Marcellus shale cores. The thin sections were characterized
using synchrotron X-ray fluorescence imaging and synchrotron X-ray
absorption spectroscopy. Fe species with different oxidation states
were identified in the maps, together with barite and Ca distribution.
The results show that ferrihydrite, as newly formed Fe(III)-bearing
precipitates, aligned well with the border of the Ca (e.g., calcite)-leaching
region in the reaction front. Some Fe-containing clay also dissolved,
but the dissolution region for the clay was not as deep as the calcite.
The reaction front is about three times deeper in the direction parallel
to the shale bedding than that perpendicular to the bedding. The Ca-leaching
region can be an index for reaction front detection for Marcellus
shale. Reactive transport modeling was conducted and the predicted
Ca-leaching border aligns well with ferrihydrite precipitation, consistent
with the experimental observation. The carbonate mineral dissolution
can be crucial to promote fluid access into the shale matrix. Together
with our previous study on the shale reactive surface, this follow-up
study showed a similar Ca-leaching region and Fe(III) precipitate
distribution in the matrix reaction front regardless of barite precipitation
on the surface, indicating that the barite coatings on the surface
may not pose a significant impact on reactive transport at the shale–fluid
interface.
“…In this study, a microcontinuum reactive transport model was used to illustrate the mineral reaction front migration and test the impacts of matrix properties. The reactive transport model has been detailed in previous studies, ,− and the simulation setup for this study is described here.…”
Hydraulic fracturing of shale reservoirs resulted in
significant
opportunities for increased oil and gas production in the United States.
Rock–fluid interactions can cause mineral dissolution and precipitation
reactions that lead to permeability changes in the shale matrix, which
ultimately may affect transport pathways and hydrocarbon production.
Understanding the distribution of secondary precipitates, such as
barite and Fe(III) (hydro)oxides, and cation leaching at the rock–fluid
interface is an important step to further investigate how these geochemical
processes can change permeability and transport pathways. In this
study, thin sections of the fracture-matrix interface were made from
reacted Marcellus shale cores. The thin sections were characterized
using synchrotron X-ray fluorescence imaging and synchrotron X-ray
absorption spectroscopy. Fe species with different oxidation states
were identified in the maps, together with barite and Ca distribution.
The results show that ferrihydrite, as newly formed Fe(III)-bearing
precipitates, aligned well with the border of the Ca (e.g., calcite)-leaching
region in the reaction front. Some Fe-containing clay also dissolved,
but the dissolution region for the clay was not as deep as the calcite.
The reaction front is about three times deeper in the direction parallel
to the shale bedding than that perpendicular to the bedding. The Ca-leaching
region can be an index for reaction front detection for Marcellus
shale. Reactive transport modeling was conducted and the predicted
Ca-leaching border aligns well with ferrihydrite precipitation, consistent
with the experimental observation. The carbonate mineral dissolution
can be crucial to promote fluid access into the shale matrix. Together
with our previous study on the shale reactive surface, this follow-up
study showed a similar Ca-leaching region and Fe(III) precipitate
distribution in the matrix reaction front regardless of barite precipitation
on the surface, indicating that the barite coatings on the surface
may not pose a significant impact on reactive transport at the shale–fluid
interface.
“…The ductile clay fractions in the fine-grained caprocks may also cover reactive solid surfaces, which leads to limited diffusion in the porous layers around the grains and hence limited (geo)chemical reactions [2]. This armoring phenomenon caused by clay minerals reshapes the available surface area for precipitation and dissolution (geo)chemical reactions during coupled thermo-hydro-mechanical-chemical (THMC) processes, leading to changes in the system's reactivity and reaction progress and rates [2,[85][86][87].…”
Section: Implications For Top Seal Integritymentioning
Understanding and predicting sealing characteristics and containment efficiency as a function of burial depth across sedimentary basins is a prerequisite for safe and secure subsurface storage. Instead of estimators and empirical relationships, this study aimed to delineate data-driven variability domains for non-cemented fine-grained clastic caprocks. Constant rate-of-strain uniaxial compression experiments were performed to measure changes in properties of brine-saturated quartz–clay mixtures. The binary mixtures were prepared by mixing quartz with strongly swelling (smectite) and non-swelling (kaolinite) clays representing end-member clay mineral characteristics. The primary objective was to evaluate the evolution of mudstone properties in the first 2.5 km of burial depth before chemical compaction and cementation. By conducting systematic laboratory tests, variability domains, normal compaction trends, and the boundaries in which characteristics of fine-grained argillaceous caprocks may vary were identified, quantified, and mathematically described. The results showed distinct domains of properties, where kaolinite-rich samples showed higher compressibility, lower total porosity, higher vertical permeability, and higher Vp and Vs. Two discrepancies were discovered in the literature and resolved regarding the compaction of pure kaolinite and the ultimate lowest porosity for quartz–clay mixtures. The present experimental study can provide inputs for numerical simulation and geological modeling of candidate CO2 storage sites.
“…26 Through this method, they revised Archie's law, for effective diffusivity in a porous medium, to account for the clogging effect explicitly. In more recent work, Deng et al 27 used a probabilistic nucleation with microcontinuum approach to precipitation to fit dissolution−precipitation experiments.…”
Nucleation
and growth processes of minerals and other crystals
can significantly affect one another due to the transport limitations
and local depletion of reactive ions in the solution. Most numerical
models and experimental measurements have typically focused on either
growth or nucleation, but not both. In this work, we incorporate a
heterogeneous nucleation process based on classical nucleation theory
into a microcontinuum model that implements the Darcy–Brinkman–Stokes
approach to study the interplay between nucleation and crystal growth
on a substrate in diffusive systems. We demonstrate how the Damköhler
number (reaction rate) and nucleation rate prefactor change the effective
nucleation rate on a substrate. Higher surface growth rates deplete
the solute concentration around the nuclei that appear initially on
the substrate, creating islands that screen against further nucleation.
The model predicts that measured nucleation rates may be affected
by the history of crystal nucleation on the substrate. In the extreme
case of high growth rates relative to diffusion, it predicts that
the rate of subsequent nucleation is limited by reactant depletion.
We introduce a nondimensional number α to represent the relation
between surface propagation rate during growth and the heterogeneous
nucleation rate. We show that it is important to control Damköhler
number and α to achieve similar precipitation regimes at different
reaction and nucleation rates. We suggest that the observed universality
can guide the interpretation of experimental results on nucleation
rates, since matching experiment can be achieved by tuning transport,
reaction, and nucleation parameters simultaneously. In addition, we
show how the bulk solution concentration affects the structure and
topology of precipitation on a substrate.
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