Carbon Dioxide Injection in Carbonate Reservoirs - A Review of CO 2-Water-Rock Interaction Studies
Carbon Dioxide Injection in Carbonate Reservoirs - A Review of CO 2-Water-Rock Interaction Studies
Carbon Dioxide Injection in Carbonate Reservoirs - A Review of CO 2-Water-Rock Interaction Studies
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Abstract: Carbon dioxide injection in geological formations is currently a common procedure in several
reservoirs worldwide. More recently, it has been considered a permanent storage solution, avoiding
emission to the atmosphere from large industrial sources. Also, it is largely employed in the oil & gas
exploration industry, for enhanced oil recovery (EOR) operations. However, it is a known fact that
injection of large amounts of CO2 into geological reservoirs may lead to a series of alterations due to
chemical and physical interactions with minerals and fluids, especially in carbonate or carbonate-rich
reservoirs. Experimental and numerical models have been employed in many studies in the past, to
investigate these effects on the geological environment. So far, most of these studies focused on
siliciclastic formations, whereas carbonate reservoirs, which are known to be much more chemically
reactive when interacting with CO2 , were much less investigated. We present a review of experimental
and numerical models that have been employed for studying CO2 -water-rock interactions, and their
application to the investigation of the impact in carbonate reservoir quality and integrity caused by the
injection of carbon dioxide. C 2017 Society of Chemical Industry and John Wiley & Sons, Ltd.
Keywords: water-rock interactions; carbon dioxide; carbonate reservoir; carbon capture and storage
Introduction aquifers, and depleted oil and gas fields or coal beds,
has become widely accepted as an important solution
Injection of carbon dioxide in geological media has to reducing CO2 emissions to the atmosphere.3–5 Once
been a common practice in the oil & gas industry since injected underground, CO2 can be retained or trapped
the 1970s, as a means of improving the oil/gas recovery in the sub-surface, by overlying impermeable
rates (a method known as tertiary or enhanced oil formations (physical trapping),6 as immovable droplets
recovery (EOR)).1 CO2 injection, often alternated with in the rock pores (residual trapping),7 as a dissolved
water, typically reduces oil viscosity and enhances oil species in the aqueous phases (solubility trapping),8,9
recovery, with up to 40% of residual oil left after or as a solid phase – mostly as carbonates (mineral
conventional operations (primary and secondary) trapping).6 Mineral trapping is considered the most
recovery.2 More recently, the idea of capturing CO2 stable and permanent form, although it is believed to
from large industrial sources and storing it in act in a much longer time scale due to the slow reaction
appropriate geological formations, such as saline kinetics and/or unfavorable conditions to precipitate
Correspondence to: Rodrigo S. Iglesias, Institute of Petroleum and Natural Resources (IPR), Pontifical Catholic University of Rio Grande do Sul
(PUCRS) – Av. Ipiranga 6681, Building 96J, Porto Alegre – RS, Brazil.
E-mail: [email protected]
Received December 8, 2016; revised March 1, 2017; accepted May 9, 2017
Published online at Wiley Online Library (wileyonlinelibrary.com). DOI: 10.1002/ghg.1693
C 2017 Society of Chemical Industry and John Wiley & Sons, Ltd. Greenhouse Gas Sci Technol. 0:1–14 (2017); DOI: 10.1002/ghg 1
TA Siqueira et al. Review: Carbon dioxide injection in carbonate reservoirs – a review of CO2-water-rock interaction studies
carbonates.4,6,10 Geological media can store oil and gas properties during CO2 injection in connection with
for millions of years; therefore it can be assumed that EOR and CO2 sequestration efforts.24 CO2 dissolution
these are stable for storage of CO2 in a similar way.3,11 in the formation water is a fast process (from minutes
Carbonate reservoirs are attractive CO2 sequestration to hours) that quickly lowers the pH of the aqueous
options, as the majority of the world’s oil reserves (ca. phase and changes the distribution of many dissolved
60%) are held in these types of rocks (especially in the species.19,25 CO2 solubility in brine can be quantified
Middle East), therefore being an interesting storage by models based on experimental data,26,27 and
target when combined with EOR operations.12 dissolved CO2 will initiate a series of geochemical
Furthermore, the recently discovered deep-water oil reactions with brine and rock-forming minerals that
fields in the South Atlantic Ocean along the Brazilian are more complicated and less well-constrained.19,21
coast (known as the Pre-Salt cluster) is formed by Some of the reactions could be beneficial by helping to
carbonate formations. CO2 injection in these reservoirs chemically trap the CO2 as dissolved species or by
is already taking place, for EOR purposes, in the Lula forming carbonate minerals; other reactions may be
field (Santos Basin), using the CO2 stripped from the damaging to the reservoir and seal integrity by
Pre-Salt reserves, which have high CO2 content.12,13 dissolving rock-forming minerals.6,28–30
However, carbonate minerals are very reactive 14 and The chemical reactions initiated by CO2 dissolution
usually form very heterogeneous reservoirs,15 and in reservoir aqueous fluids is well known and described
therefore are very likely to suffer significant alterations herein.31 Initially, the dissolution causes a significant
with CO2 injection, which may affect integrity, acidification of the medium by formation of carbonic
injectivity, and consequently, storage safety.16 acid:
Furthermore, storage capacity can be affected with CO2 + H2 O ↔ H2 CO3 (1)
changes in the rock porosity and permeability.17,18
Thus, the investigation of CO2 -water-rock interactions This acid dissociates generating bicarbonate ions
and their impact in this type of reservoirs is extremely (HCO3 − ):
important. This review aims to evaluate the main H2 CO3 + H2 O ↔ H3 O+ + HCO− (2)
3
experimental and numerical modeling studies focusing
on these interactions in carbonate reservoirs, The dissolved bicarbonate species react with divalent
considering the growing interest in using CO2 for cations to precipitate carbonate minerals, provided the
enhanced oil recovery as well as for geological acidity of the aqueous media is adequate (neutral to
sequestration in such reservoirs. alkaline pH) – otherwise the species stay in solution.
The formation of calcium, magnesium or iron
Interactions between CO2 and carbonates at higher pH is expected to be the primary
means by which CO2 is fixed in a permanent stable
geological media form.10
Several physicochemical alterations are triggered by
HCO−
3 + Ca
2+
↔ CaCO3 + H+ (3)
massive injections of CO2 in the geological media,
affecting both reservoir and caprock for large distances
HCO−
3 + Mg
2+
↔ MgCO3 + H+ (4)
(kilometers) and long periods (several years).5,19 In
carbonate media, these alterations are usually fast and
HCO−
3 + Fe
2+
↔ FeCO3 + H+ (5)
may have important consequences during injection
and storage processes.20 Dissolved divalent cations may already be present in
When injected in a reservoir, carbon dioxide leads to the formation water, or originated via dissolution of the
a disequilibrium of both fluid chemistry and pore primary rock minerals by CO2 -acidified water
pressures within the reservoir and caprock.21 In the injection.19,28 The extent of mineral trapping is directly
vicinity of injection wells, CO2 dissolves into resident related to the quantity of these cations available in
reservoir fluids, which lowers the pH, usually resulting solution and the medium pH.6
in mineral dissolution and alteration of porosity and Other carbonates with alkaline metals, such as the
permeability.22,23 Quantifying these processes and their sodium-aluminum carbonate hydroxide dawsonite
influence on the hydraulic properties of the reservoir is (NaAlCO3 (OH)2 ) have been suggested as a possible
critical to understanding the evolution of transport precipitation product of CO2 injection in reservoirs in
2
C 2017 Society of Chemical Industry and John Wiley & Sons, Ltd. Greenhouse Gas Sci Technol. 0:1–14 (2017); DOI: 10.1002/ghg
Review: Carbon dioxide injection in carbonate reservoirs – a review of CO2-water-rock interaction studies TA Siqueira et al.
modeling studies, following dissolution of albite and carbonate minerals in their rock matrix, and their
aluminosilicates (such as kaolinite).32–34 Some reactivity can be significantly different.
experiments indicate that dawsonite stability is
dependent on a high CO2 pressure and pH, quickly
dissolving following pressure decrease, leading to
Experimental studies
precipitation of kaolinite.35,36 Experimental methods and characterization
In carbonate formations, the main cause of porosity techniques to investigate CO2 -water-rock interactions
and permeability reduction is the precipitation of are well known and often rely on batch and
CaCO3 and NaCl, which occurs by increase of pH and flow-through reactor systems. These methods are fully
the concentration of Cl− ions in the brine by described in a comprehensive study published recently
desiccation, respectively.37 Brine desiccation is a by Kaszuba et al.45 and references therein.
known effect that is likely to occur near the injecting Among the major studies related to geologic carbon
well. As CO2 is injected in dry state, once in contact sequestration, those from Gunter et al.10 and Kaszuba
with the reservoir brine, H2 O is partially dissolved in et al.37 stand out as being the first ones to focus on the
the dense CO2 . With high injection rates, substantial alterations of the target reservoir due to interactions
amounts of H2 O can transfer to the CO2 phase, thereby with CO2 at reservoir conditions. These studies
concentrating the aqueous species in the brine.37 This evaluated the effect of more reactive conditions (higher
brine concentration subsequently induces kinetically temperature) on mineral reactivity, compared results to
fast precipitation reactions of minerals such as numerical models and identified key effects such as
carbonates, sulfates, and evaporates.38 The mechanisms brine desiccation effects from supercritical CO2 .
by which a precipitate reduces the permeability are Several experimental studies have been published
much less understood and difficult to predict than aiming to understand the influence of CO2 -fluid-rock
dissolution effects, as there are several factors that interactions and precipitation of minerals in a system
determine whether precipitation occurs within the that simulates the geological storage in saline aquifers
pore space or throats. Also, the precipitated material and oil/gas fields. The potential application of
may either remain in place or be transported geological storage of CO2 have been studied and
elsewhere, depending on flow conditions.39 improved over the years.34,43,46–50
The connection between chemical interactions and Most of the earlier studies have investigated
their impact on porosity and permeability is a known siliciclastic reservoirs, and only more recently have
issue with a difficult resolution. Nonetheless, it has carbonate reservoirs started to receive more attention.
attracted attention, as this correlation is crucial to This is unsurprising, as carbonate formations are much
understand the impacts of geochemical reactions more reactive to CO2 -induced acidic media, as
induced by CO2 .40,41 Therefore, previous opposed to siliciclastic formations, for which most
characterization of any storage site is essential prior to experimental studies have shown negligible changes
the injection stage.19,42 from short-term interactions with CO2 , usually
Typically, the study of geochemical interactions restricted to carbonate cement in the
between CO2 , fluid and minerals in a reservoir or samples.19,40,43,51,52 Here we reviewed some of the most
caprock is mostly based on laboratory experiments as relevant experimental studies on carbonate reservoir
well as the use of numerical modeling tools.43 interactions with CO2 published until now.
Particularly, pore-scale modeling of reactions induced One of the earliest works on CO2 injection
by CO2 and experimental characterization of changes experiments in carbonate reservoirs was published by
in geometry of the pore space in geological storage Luquot and Gouze in 2009, conducting a study on the
conditions seem promising to improve the behavior of limestone reservoirs from the Mondeville
understanding of the impact of these interactions.19 formation of Middle Jurassic age (Paris Basin, France),
Further understanding can also be obtained through interacting with injected CO2 , through a series of four
the investigation of existing natural CO2 reservoirs, flow-through experiments.40 The experiments aimed
studying the characteristics and diagenesis of these to simulate mass transfer occurring near the injection
formations.44 These studies, although important for the well and at increasing distances from the injection well.
understanding of these reservoirs, were not included in The expected patterns of rock dissolution controlled
this review, as these natural reservoirs may not include by the composition of the injection fluid can be
C 2017 Society of Chemical Industry and John Wiley & Sons, Ltd. Greenhouse Gas Sci Technol. 0:1–14 (2017); DOI: 10.1002/ghg 3
TA Siqueira et al. Review: Carbon dioxide injection in carbonate reservoirs – a review of CO2-water-rock interaction studies
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C 2017 Society of Chemical Industry and John Wiley & Sons, Ltd. Greenhouse Gas Sci Technol. 0:1–14 (2017); DOI: 10.1002/ghg
Review: Carbon dioxide injection in carbonate reservoirs – a review of CO2-water-rock interaction studies TA Siqueira et al.
Figure 2. XCMT images before and after reaction, for vuggy samples reacted at pCO2 (a)
3 and (b) 2 Mpa, (c) 1 and (d) 0.5 Mpa for marly samples. Pore space both prior and
post-reaction is shown in gray in XCMT image.54
The carbonate dissolution behavior in both samples experiments were carried out at ca. 14 Mpa of pore
fits general rate expressions that link the dissolution to pressure and 60°C and flow rates ranging from
thermodynamics (i.e., dependence on rate constant 0.1 mL/min to 20 mL/min.
and distance from equilibrium terms). Additionally, The authors observed that the presence of fractures
the calcite reaction rate constant was about 17 times does not significantly alter the wormhole formation
greater than that of dolomite during reaction.55 process. The results showed that a higher flow rates,
The effective mass transfer rates of calcite and dissolution of the porous media results in a branched
dolomite were observed in the marly dolostone growth pattern, whereas the presence of a preexistent
samples. The final measurements of calcite mass fracture provides a referential flow path that grows
transfer rates were approximately two times faster than uniformly without indication of branching in the
rates dolomite. Mass transfer rates measured in vuggy porous matrix.
experiments were much more variable. Calcite mass In a study published in 2014, Luquot et al. performed
transfer rates reached levels of 40–60% of the a series of reactive coreflood experiments reproducing
maximum values after the wormholes were reservoir conditions (100°C and 12 MPa), injecting
established.54,56,57 CO2 -rich brine in oolitic limestone (99% calcite)
It was observed in this study that the heterogeneity of samples.41 Aiming to understand the dissolution
pore space of these carbonate rocks exerted a strong regimes both near and far from the injection well,
influence on the type of dissolution and the resulting experiments were conducted at different CO2 partial
relationship between porosity and permeability. Pore pressures (varying from 0.034 MPa to 3.4 MPa).
space distribution more homogeneous led to carbonate Results were evaluated combining XCMT imaging
mass transfer rates sustained steady-state, resulting in techniques and pore network geometry analysis
stable dissolution fronts, causing only small changes in obtained from the images.
permeability. Analysis of the results show a dependence of
These observations suggest specifically that the dissolution pattern with CO2 injection rate (partial
formulation carbonate kinetic rate does not requires pressure), which is linked to the medium acidity –
additional dependency of pH or pCO2 may be higher rates (more acidic media) induce dissolution
applicable, when the variation of the pH is relatively localization, while lower rates result in more
low.54 homogeneous dissolution. By quantifying the changes
A study conducted by Elkhoury et al. in 2013 verified in pore connectivity from the pore network skeleton
the dissolution and deformation in fractured analysis, the authors observed that higher injection
carbonates rocks caused by flow of CO2 -rich brine rates increase the number of skeleton branch tips after
under reservoir conditions.58 The rock samples used in the dissolution experiment, which means a growth of
these experiments were obtained from the lower preferential flow paths, increasing connectivity and
Midale Vuggy formation of the Weyburn field. The permeability. These alterations may favor CO2
C 2017 Society of Chemical Industry and John Wiley & Sons, Ltd. Greenhouse Gas Sci Technol. 0:1–14 (2017); DOI: 10.1002/ghg 5
TA Siqueira et al. Review: Carbon dioxide injection in carbonate reservoirs – a review of CO2-water-rock interaction studies
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C 2017 Society of Chemical Industry and John Wiley & Sons, Ltd. Greenhouse Gas Sci Technol. 0:1–14 (2017); DOI: 10.1002/ghg
Review: Carbon dioxide injection in carbonate reservoirs – a review of CO2-water-rock interaction studies TA Siqueira et al.
authors suggest a good efficiency for geological of the carbonate matrix can be dangerous because it
sequestration in carbonate sedimentary rocks. The could induce fractures and activate faults in the
following ideal conditions for CO2 storage are reservoir. Hence, geochemical simulation may also be
recommended by the authors:14 (i) carbonate necessary to model the possible mineral dissolution
reservoirs of dolomite or magnesite, especially far from and precipitation processes near the injection wells.
the CO2 injection front; (ii) presence of calcite near the Geochemical modeling of CO2 -water-rock
vicinity of the injection well, so as to provide a high interactions can be divided into two approaches. One is
concentration of HCO3 − and pH greater than 5; (iii) a the calculation of the thermodynamic equilibrium of
temperature between 100°C to 150°C; and (iv) a partial the CO2 -water-rock system. With this calculation, it is
pressure of CO2 of 50 atm or higher. possible to estimate the solubility of CO2 in the
However, according to Peng et al.62 and Wunsch formation fluid, as well as mineral saturation states at
et al.63 CO2 -promoted dissolution can play a significant equilibrium. A second approach is to model the
role in kinetics of calcite dissolution rates at kinetics of dissolution and precipitation of the minerals
temperatures from 50°C to 100°C and partial pressures with time. Most studies employ a generic rate law
of CO2 from 60 to 138 bar. In this study, it was based on transition state theory (TST) derived by
observed that the calcite dissolution rates in the Lasaga67 for these processes, which depends on a rate
CO2 -H2 O system increased with the increase of CO2 constant, the specific reactive surface of the mineral,
partial pressure.63 It is important to observe that the temperature, pH, and deviation from the equilibrium
experimental system specifically designed by Peng state. Although specific rate laws for relevant minerals
et al.62 for these experiments is different and it was used have been used in some cases, sensitivity studies have
to eliminate mass–transfer resistance and to access the shown that results are not significantly affected.19,24,68,69
reaction rates under reactive surface-controlled regime
at far-from equilibrium conditions 62–64
Some experimental simulations were performed by Numerical modeling studies
Montes-Hernandez in 2016 to evaluate how a heating As in the case of experimental modeling investigations,
step promotes the rapid formation of dolomite under only a few studies of numerical modeling of
alkaline conditions of high carbonate content through CO2 -water-rock interactions in geological reservoirs
dissolution-precipitation reactions, to determine how have been developed focused specifically in carbonate
carbonates can dissolve or precipitate.59 It was reservoirs, with the majority being applied to
observed that alkaline conditions reduce the hydration siliciclastic formations.68,70–73 It is essential that
of magnesium, increasing its incorporation into calcite modeling studies applied to carbonate reservoirs
or the direct formation of dolomite. Due to the heating include chemical changes (geochemical and reactive
step, dolomitization can be achieved within a few days. transport models), due to the fast kinetics of
The temperature has a significant influence on the dissolution and precipitation of carbonate minerals.64
kinetics of dolomitization, the extension of the reaction Changes in the porosity and permeability are likely to
and mineral composition.37,50,59,65 be significant in most cases, due to the high reactivity
of carbonate minerals. These alterations of the porous
media due to injection of acid fluids and the conditions
Numerical modeling for formation of wormholes and their structural
Numerical modeling plays an important role in the features has been the object of some theoretical
investigation of the interactions between carbon investigations in the past years.74–81
dioxide and the reservoir. It allows to estimate, for Among the most relevant papers published of studies
instance, the consequences of a large-scale CO2 of numerical modeling of CO2 -rock-fluid system in
injection to the reservoir and caprock in a geological carbonate reservoirs, we can cite those by the groups of
time scale, thus being complementary to the laboratory IFP and BRGM on the Dogger aquifer in the Paris
experiments.66 Basin,30,82,83 the experimental and numerical modeling
Chemical reactions can play an important role in the investigation by Izgec et al. using the reservoir
injection phase, particularly in carbonate reservoirs simulator STARS (Computer Modelling Group),84,85
that dissolve more rapidly with the acidification of the and a study by researchers at Shell together with Tianfu
brine by dissolution of CO2 . An extensive dissolution Xu of Lawrence Berkeley National Laboratory (LBNL)
C 2017 Society of Chemical Industry and John Wiley & Sons, Ltd. Greenhouse Gas Sci Technol. 0:1–14 (2017); DOI: 10.1002/ghg 7
TA Siqueira et al. Review: Carbon dioxide injection in carbonate reservoirs – a review of CO2-water-rock interaction studies
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C 2017 Society of Chemical Industry and John Wiley & Sons, Ltd. Greenhouse Gas Sci Technol. 0:1–14 (2017); DOI: 10.1002/ghg
Review: Carbon dioxide injection in carbonate reservoirs – a review of CO2-water-rock interaction studies TA Siqueira et al.
Figure 5. Changes in porosity (a) and permeability (b) in a caprock after 1000 years of
interaction with CO2 injected.30
C 2017 Society of Chemical Industry and John Wiley & Sons, Ltd. Greenhouse Gas Sci Technol. 0:1–14 (2017); DOI: 10.1002/ghg 9
TA Siqueira et al. Review: Carbon dioxide injection in carbonate reservoirs – a review of CO2-water-rock interaction studies
Figure 7. Changes of calcite (a) and dolomite (b) of the reservoir after 1 year of injection.94
Figure 8. Simulated (lines) and experimental data (symbols) from the dolomite core-flood
study by Luhmann et al. 52
Hao et al. complemented their experimental work 54 continuum model results were capable of reproducing
with a numerical modelling simulation of the the core flood dissolution patterns quite well (Fig. 9),
experiments using a 3D continuum-scale reactive provided rate constants for reaction kinetics and
transport model57 of core flood experiments, with two power-law exponents for the porosity-permeability
samples from the Weyburn-Midale CO2 Monitoring relationship were properly constrained by calibration
and Storage Project, a marly dolostone and a vuggy with experimental data.
limestone. Simulations were carried out using the The study presents an interesting analysis of the
NUFT code (Nonisothermal Unsaturated-Saturated relationship between formation of dissolution ‘fingers’
Flow and Transport code).96 The model grid and initial and porosity contrast within carbonate (calcite and
properties (porosity, permeability, and surface area dolostone) samples, indicating that the macroporosity
distribution) were built based on tomographic images and, more importantly, a higher porosity contrast in
of the core and microscopy characterization data. The pore-size distribution, are the main factors leading to
10
C 2017 Society of Chemical Industry and John Wiley & Sons, Ltd. Greenhouse Gas Sci Technol. 0:1–14 (2017); DOI: 10.1002/ghg
Review: Carbon dioxide injection in carbonate reservoirs – a review of CO2-water-rock interaction studies TA Siqueira et al.
C 2017 Society of Chemical Industry and John Wiley & Sons, Ltd. Greenhouse Gas Sci Technol. 0:1–14 (2017); DOI: 10.1002/ghg 11
TA Siqueira et al. Review: Carbon dioxide injection in carbonate reservoirs – a review of CO2-water-rock interaction studies
Acknowledgments 13. Ketzer JM, Machado CX, Rockett GC and Iglesias RS (eds),
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The authors would like to thank PETROBRAS S.A. and EDIPUCRS, Porto Alegre, Brazil (2015).
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