Environ. Sci. Technol.

2008, 42, 27422747

in the case for the cap-rocks that have confined buoyant oil
Reservoir Engineering To Accelerate and gas for geologic time scales.
the Dissolution of CO2 Stored in The CO2 injected into a deep aquifer is typically 1040%
less dense than the resident brine. Driven by density contrasts
Aquifers CO2 will flow horizontally spreading under the cap-rock and
may flow upward, leaking through any high permeability
zones or artificial penetrations such as abandoned wells.
YURI LEONENKO AND DAVID W. KEITH*
After injection, free-phase CO2 (gas or supercritical fluid)
Energy and Environmental Systems Group, Institute for slowly dissolves in the brine (7). The resulting CO2-rich brine
Sustainable Energy, Environment and Economy, University of is slightly denser than the preexisting brine, making it
Calgary, 2500 University Drive, Calgary AB, Canada T2N 1N4
negatively buoyant thus eliminating the most important
driving force for upward migration.
Received June 27, 2007. Revised manuscript received Natural convection processes can accelerate the dissolu-
November 28, 2007. Accepted November 29, 2007. tion beyond that which would occur with diffusion alone.
Convection may occur when dense CO2-rich brine formed
under the bubble of free-phase CO2 overlies lower density
undersaturated brines. The time scale for the onset of
It is possible to accelerate the dissolution of CO2 injected convection can range from years to centuries. The time
into deep aquifers by pumping brine from regions where it is needed for the CO2 to dissolve completely is typically much
undersaturated into regions occupied by CO2. For a horizontally longer, on the order of 102-104 years depending on the vertical
confined reservoir geometry, we find that it is possible to permeability (710).
dissolve most of the injected CO2 within a few hundred years By eliminating the role of buoyancy in driving possible
at an energy cost that is less than 20% of the cost of leakage of CO2, the dissolution of CO2 in brines confers a
compressing the CO2 to reservoir conditions. We anticipate significant advantage to aquifers with respect to security of
that use of reservoir engineering to accelerate dissolution can storage. Considering both aquifers and oil and gas reservoirs
reduce the risks of CO2 storage by reducing the duration that contain water as wet reservoirs, it is now plausible to
argue that, contrary to earlier assumptions, such systems
over which buoyant free-phase CO2 is present underground.
offer both greater capacity and, due to dissolution, superior
Such techniques could simplify risk assessment by reducing storage security than do dry reservoirs in which CO2 would
uncertainty about the long-term fate of injected CO2, and could remain buoyant indefinitely.
expand the range of reservoirs which are acceptable for As a conceptual framework for assessing storage security,
storage. we adopt the view that the only relevant risk of leakage arises
from mobile free-phase CO2, that is, CO2 that remains in the
gas (or supercritical fluid) phase and which is not immobilized
Introduction by residual gas trapping. Storage performance thus depends
Geologic storage of CO2 is an important tool for managing on two factors: (i) the likelihood that free-phase CO2 will leak
global CO2 emissions (1). Industrial scale CO2 storage projects out of the reservoir or alternatively the time scale over which
now operational or in design phase provide strong empirical significant leakage is expected to occur and (ii) the rate at
support for the view that CO2 storage can be implemented which free-phase CO2 is immobilized by residual gas trapping,
in a safe manner and at acceptable cost. Nevertheless, dissolution in the reservoir fluids, or subsequent geochemical
significant uncertainties remain regarding the risks, cost, and reactions. Storage security can be increased either by reducing
availability of underground storage at the scales necessary the probability of leakage or by increasing the rate at which
for this technology to play a significant role in managing CO2 is immobilized within the aquifer. Hereafter, we use
global emissions. Managing one-third of current global CO2 reservoir to describe a CO2 storage site which might be an
emissions with carbon capture and storage (CCS), for aquifer or a hydrocarbon reservoir with significant water
example, would require disposal of CO2 at an average rate saturation. We use brine to denote aqueous fluids of any
of 15 km3/year at reservoir conditions, a rate approximately salinity.
5000 times the total volume of CO2 currently injected in In contrast to much of the previous work on geologic
dedicated CCS projects. This quantity is similar to the scale storage which has focused on site selection, monitoring, risk
of the entire current oil and gas industry, the technological assessment, or remediation, our focus is on active reservoir
foundation for CO2 storage, which now produces 5 km3/ engineering to accelerate dissolution and also to reduce the
year of oil and 15 km3/year of gas at reservoir conditions maximum pressure within the reservoir. Here we use
(2). physically based scaling arguments and numerical simula-
As assessments of geologic storage began in the early tions to assess the technical and economic feasibility of
1990s, attention naturally focused on oil and gas reservoirs accelerating the dissolution of CO2 in aquifers.
(3, 4). Although it was recognized that deep aquifers offered
very large potential storage capacity, they were typically
Methods To Accelerate Mixing
viewed as offering less certain and less secure storage than
did oil and gas reservoirs (5, 6). Less certain because deep Dissolution of CO2 in aquifer brine could, in principle, be
aquifers have seen far less exploration than oil and gas accomplished either within the reservoir or at the surface.
reservoirs due to the absence of an economic incentive and Surface. Surface, or ex situ, dissolution could be achieved
less secure because the confining formations aquitards or within a pipeline operating at the pressure of the target
cap-rocks have not been proven to hold buoyant fluids as reservoir into which CO2 is to be injected, (Figure 1, left panel).
The generation of CO2 bubbles or droplets sufficiently small
* Corresponding author phone: (403) 220-6154; e-mail: keith@ to achieve rapid dissolution might rely on turbulent two-
ucalgary.ca. phase flow within the pipe (11).
2742 9 ENVIRONMENTAL SCIENCE & TECHNOLOGY / VOL. 42, NO. 8, 2008 10.1021/es071578c CCC: $40.75 2008 American Chemical Society
Published on Web 02/01/2008
 CO2 1

)
H2O R

The solubility of CO2 in brine at typical reservoir conditions

(pressure 100150 bar; temperature ) 5075 C; salinity
010% of solid by weight) is about 37% by mass. So for R
) 5% at 100% dissolution efficiency (
) 1) the mass of brine
would need to be 20 times the mass of CO2.

Numerical Simulations
There is no doubt that sufficiently aggressive brine circulation
can accelerate CO2 dissolution in aquifers; the question is,
can acceleration be accomplished with sufficiently low energy
cost and high efficiency in realistic reservoirs with sufficiently
FIGURE 1. Schematic view of ex situ and in situ dissolution of inexpensive injection well geometries? We explored the
CO2 in reservoir brine. effectiveness with which brine injection can accelerate
dissolution in a suite of numerical experiments using
Ex situ dissolution would require energy to overcome idealized reservoir geometries in which injection rates and
pressure drops in both the mixing pipeline and the aquifer. the geometry of injection wells was varied in order to assess
Preliminary scaling analysis based on Dukler et al. (12) the sensitivity of energy cost, E, and dissolution efficiency,
suggests that the required pressure drop in the mixing
, to reservoir parameters and injection system design. The
pipeline would not be prohibitive. experiments used reservoir properties typical of aquifers that
Both in situ and ex situ dissolution require energy to drive might be available for CO2 sequestration (13).
brine flow in the reservoir. For ex situ dissolution the Figure 2 presents results from simulations of an idealized
volumetric flux of brine must be much larger than the CO2 top-hat reservoir geometry such as that shown schemati-
flux because the solubility of CO2 in brines is only a few cally in Figure 1, which one may think of as a crude
percent by mass. Within the reservoir the pressure drop and representation of an anticlinal petroleum reservoir. The
the pumping energy per unit volume are proportional to flux horizontal step in the cap rock that confines the buoyant
(Darcy flow), so the larger fluxes required for brine injection CO2 is circular with a radius of 1.2 km and thickness of 60 m.
mean larger pumping energy. For a CO2 solubility of 5%, for The closed aquifer of radius 6 km and a maximum thickness
example, the brine flow rate would be 20 times larger than of 100 m is homogeneous, isotopic, and isothermal with
the CO2 flow rate, and the pumping power required for brine permeability of 0.2 10-12 m2 (200 mD), porosity of 25%,
injection would be 400 times larger than that required for and rock compressibility of 1.45 10-5 1/bar. Initial
CO2 alone (neglecting differences in viscosity and relative conditions include temperature (50 C), pressure (150 bar),
permeability in two-phase flow). salinity (4% of NaCl by weight), water saturation (1), and gas
In Situ. If the mixing is accomplished in situ (Figure 1, saturation (0). See Supporting Information Section 1. These
right panel), then the time scales for CO2 and brine injection reservoir properties are very similar to those used in the
can be decoupled. If CO2 injection occurs over 20 years, for Berkeley Laboratory intercomparison study (14). We consider
example, and forced brine circulation over 200, then the the applicability of this idealized reservoir geometry to real
energy required for pumping brine will be about 10% of the world cases in Results and Discussion.
energy that would have been required to inject fully saturated Simulations used a Computer Modeling Group Ltd. (CMG)
brine in which CO2 had been dissolved ex situ assuming the (15). Commercial simulator which was validated against
same amount of brine is required. The decoupling of time TOUGH-2 simulator (16); the maximum differences on
scales is the primary advantage of in situ dissolution, while Problem 3 of the intercomparison study (14) were 3, 5, and
the primary disadvantage is the difficulty of ensuring that <1% for pressure, CO2 saturation, and dissolved CO2,
injected brine efficiently dissolves the CO2. respectively. The simulations in Figure 2 used a 3-D radial
Energy Cost of Accelerating Dissolution. The perfor- nonlinear grid with a resolution of 60 80 39 (radius
mance of an accelerated dissolution scheme may be judged height angle; see Supporting Information). Numerical
according to two figures of merit, the additional energy discretization was tested using various grids and the residual
required and the dissolution efficiency, defined below. discretization errors in the quantity of dissolved CO2 were
Additional Energy. Forced brine circulation uses energy less than 5% (Section 2 of Supporting Information). While it
beyond that required for a conventional CO2 capture and is common to use compositional simulators for CO2 storage
storage operation. This energy requirement is crucial to modeling, we employ a black oil simulator (CMG IMEX).
determining the overall cost of accelerating dissolution. The For a two-component problem the black oil and composi-
figure of merit, E, is the ratio of additional pumping work tional formulations are mathematically equivalent, while the
done to the additional mass of CO2 dissolved. For conven- black oil one is substantially more computationally efficient.
ience, we normalize this by 400 kJ/kg which is the ap- The black oil parameters (brine as an oil and CO2 as a gas)
proximate energy requirement to compress CO2 from stan- simulate the CO2-brine system using high-accuracy ap-
dard conditions to typical reservoir conditions (1), shown as proximations to the equation of state (17).
follows: In the results shown in Figure 2, a single circular horizontal
injection well is located directly below the cap-rock with a
pumping work (kJ) 1 radius of 1.1 km. As we have shown elsewhere (18), this choice
E )
CO2 dissolved (kg) 400 (kJ/kg) of injection well radius roughly maximizes dissolution rate
for the conditions chosen here. The circular geometry is an
Dissolution Efficiency. The second figure of merit is the artifact of the circular reservoir geometry; results for other
dissolution efficiency
, the ratio of the additional mass of well configurations are shown in the Supporting Information.
dissolved CO2 due to force of brine circulation to the mass Brine injection uses the same horizontal well, starting when
of brine circulated, normalized by solubility of CO2 in brine CO2 injection stops 20 years into the simulation. Brine is
at mean reservoir conditions, R. produced using three vertical brine producer wells placed

VOL. 42, NO. 8, 2008 / ENVIRONMENTAL SCIENCE & TECHNOLOGY 9 2743

FIGURE 2. Simulation results in a top-hat reservoir geometry. Each subplot shows 100 m in the vertical and 3.5 km in the radial
direction. The left column shows CO2 saturation, the fraction of pore volume occupied by free-phase CO2, while the right column
shows the amount of dissolved-phase CO2 in the brine. The black dot in each subplot shows the location of the injection well. The
percentages given on the CO2 saturation plots indicate the fraction of CO2 that is dissolved at the specified time. Black arrows mark
the plume of residually trapped CO2 that accelerates the onset of convection. An animated version of this simulation can be found in
Supporting Information (video file).

symmetrically 5 km from the center of the reservoir, far which is larger than the layer of saturated brine produced
enough to avoid breakthrough of high-CO2 brine during the in the base case, creating a stronger density instability and
simulations. thus a more rapid initiation of convection.
Injection of both brine and CO2 is at constant 1 Mt/year Dissolution would be slow without brine injection.
flux, while the brine production wells maintained at a Analytical results derived elsewhere (19) suggest that for the
constant bottom hole pressure allowing brine to flow to the case presented in this paper it would take 500 years for
surface without pumping. At year 20 when injection switches convection to become fully developed (to reach the maximum
from CO2 to brine, the brine wells are producing at a rate of Sherwood number) in the brine directly underneath the CO2
1.5 Mt/year (because CO2 has lower density than brine at gas-cap, resulting in the dissolution of 8% of the CO2. After
reservoir conditions) which quickly declines to match the equilibration of the brine below the gas-cap, the rate of
1Mt/year brine injection rate. The composition of injected dissolution should slow dramatically as it became limited by
brine is constant matching the initial brine composition in radial convection outward into the thinner regions of the
the reservoir which is consistent with that which would be reservoir.
produced using continuous reinjection since the CO2-rich Figure 3 presents the results for dissolution vs time for
brine does not reach the production wells during the 300 different brine injection rates (solid lines). It also shows the
year simulation period. results for the nonconfined case (dashed lines), which is
Without brine injection, 6.5% of the CO2 is dissolved during infinite reservoir with the depth of 100 m and it has the same
the 20 years of CO2 injection and only an additional 1.5% reservoir conditions as described for the confined reservoir.
dissolves over the remaining 300 years of simulation (Figure Brine injection is substantially more effective in accelerating
3), whereas with brine injection at a rate of 1 Mt/year, 71% dissolution in the confined geometry in comparison with a
of the CO2 is dissolved within 300 years. Over this period, the nonconfined one because the buoyancy force acting on the
figures of merit for additional energy and dissolution CO2 brings it into closer contact with the injected brine. In
efficiency are E ) 0.16 and
) 0.89. the case of the nonconfined reservoir, brine injection pushes
With or without brine injection, convection develops the CO2 away from the injection point reducing the ef-
within the brine during the later half of the simulation driven fectiveness of further injection.
by the density contrast that arises when dense CO2-rich brine The dissolution rate is proportional to the brine flow rate
created by contact with the free-phase CO2 overlie the less- at the beginning of injection, but the rate declines with time
dense unsaturated brine. Interestingly, convection is stronger due to the declining thickness of the CO2 plume which reduces
in the case with brine injection. This appears to be due to the contact between injected brine and CO2 (Figure 3). At
the fact that in the injection case the residually trapped CO2 first, the brine flows downward through a two-phase region
left below the retreating bubble of free-phase CO2 (see arrows where it can be efficiently mixed with the existent free-phase
in Figure 2, left panel) produces a plume of saturated brine CO2. The knee in the cumulative dissolution curves occurs

2744 9 ENVIRONMENTAL SCIENCE & TECHNOLOGY / VOL. 42, NO. 8, 2008

FIGURE 3. Dissolved fraction as a function of time. Solid lines show results from the top-hat geometry, while dashed lines are for an
infinite slab geometry. Brine injection rates are indicated in megatons per year. Arrows denote the knee in the curves discussed
in the text.
when the CO2 saturation in the downward flowing brine
declines to zero, so that the brine flows downward through
a single (brine) phase region. Dissolution then depends on
diffusion of CO2 from the surrounding two-phase region into
the brine jet reducing dissolution efficiency. For the 2 Mt/
year brine injection,
drops from 0.9 at simulation year
130 to 0.15 after the knee in the curve at year 150. Comparison
of the 1 and 3 Mt/year cases in Figure 3 shows that lower
injection rates may provide more efficient dissolution. The
uppermost curve shows results with an injection rate that
declines with time to increase the dissolution rate while
maintaining efficiency.

Results and Discussion

Forced dissolution is applicable to a range of reservoir
geometries. The infinite slab geometry is a particularly
unfavorable case for accelerating dissolution because most
water bypasses the unconfined CO2 plume, resulting in high FIGURE 4. Pressure field in the top-hat reservoir geometry
E and low
. The top-hat case presented here is more showing location of the brine production wells. Data are
favorable, but it is by no means the most favorable circum- plotted to a maximum radius of 6 km. Data are for the bottom of
the reservoir at the end of the CO2 injection (20 years).
stance. More favorable conditions for accelerating dissolution
would include (i) a geometrically similar reservoir in which
the CO2 gas-cap has a higher thickness-to-width ratio, (ii) a available storage capacity. In a closed (volumetric) reservoir
geometry in which the cap-rock had an anticlinal curvature without brine production the bottom hole pressure may
or a pronounced dip caped by an unconformity; or finally,
approach fracture pressure forcing CO2 injection to stop long
(iii) a reservoir with higher permeability.
before the available storage capacity has been utilized. In
In results presented elsewhere we have obtained high
the Western Canada Sedimentary Basin, for example, fracture
dissolution efficiencies and low dissolution energy using
several different reservoirs and injection well geometries and pressure varies from 1.5 to 3 times hydrostatic pressure (21).
different reservoir anisotropy and inhomogeneity (18) (see Taking the lower limit and using the top-hat reservoir
also Section 4 of Supporting Information). Similar results described above, CO2 injection would need to be terminated
are obtained in infinite-acting reservoir geometries so long as early as year 7 when the bottom hole pressure exceeded
as there is a step in the cap-rock to provide some horizontal 22.5 MPa. Whereas when brine production is allowed, the
confinement of the CO2 (18). Use of cyclic injection of water maximum bottom hole pressure reached at the end of CO2
or CO2 can also improve the efficiency of dissolution (18, 20). injection (model year 20) is under 19 MPa. Figure 4 shows
The consistency of results across reservoir and injection well the pressure field at the bottom of the reservoir at year 20.
geometries suggests that similar engineering techniques
could be applied to real-world reservoirs. While the optimal In addition to increasing the effective storage capacity,
geometry would depend on the specifics of the target reservoir brine management may reduce the risk of leakage by reducing
our results suggest that for a reservoir with relatively sharp the driving force for the CO2 transport (22) and by reducing
horizontal confinement, use of a horizontal well (or wells) geomechanical stresses that might activate fractures. It also
that roughly encircle the periphery of the initial CO2 plume lowers the energy required for CO2 injection by reducing
might provide a favorable geometry. required injection pressures. In some cases, the energy saved
In addition to accelerating dissolution, brine production in CO2 injection can be more than the energy required for
enables management of reservoir pressure which can increase brine pumping to accelerate dissolution.

VOL. 42, NO. 8, 2008 / ENVIRONMENTAL SCIENCE & TECHNOLOGY 9 2745

Economics free-phase CO2 bubble to direct it away from a spill point
or a known weakness in the cap-rock.
Although the reservoir engineering necessary to accelerate Most analysis of CO2 storage has focused on site selection,
dissolution will be strongly site-specific, we nevertheless monitoring, and risk assessment. While these activities are
describe how the simulation results might be applied to a necessary for managing CO2 storage, the possibility of more
more realistic reservoir and provide a rough estimate of the active reservoir engineering such as the brine injection
costs and compare them to the costs of CO2 capture and explored here should not be ignored. Such methods might
storage in order to gauge the potential applicability of the play an important role in geologic storage for three distinct
technique. reasons. First, active reservoir engineering can reduce the
While the cylindrically symmetric reservoir geometry risk of leakage. Second, such engineering may increase
described here is of course unrealistic, the required 7 km available storage capacity by increasing the range of aquifers
total length of the horizontal injector well is roughly indicative in which CO2 can be safely stored. Third, by shortening the
of the length of a horizontal well that would be needed to time scale over which free-phase CO2 remains in the reservoir,
surround the periphery of a similar volume reservoir with a such methods might facilitate risk analysis and reduce
more realistic geometry assuming a reservoir thickness of regulatory and other uncertainties related to storing mobile
100 m which is typical of the high injectivity formations often CO2 underground for long durations.
considered for CO2 storage. There is a trade-off between the
number and length of brine production and injection wells
Acknowledgments
and the pressure drop and thus the energy and operating
costs of brine injection. The horizontal injection wells would This work was supported in part by Natural Sciences and
be drilled using a few drill pads each with two opposite Engineering Research Council of Canada and Alberta Energy
directed horizontal legs of a few kilometers (see Figure 1S in Research Institute. The authors gratefully acknowledge
contributions from Sally Benson, Olav Bolland, Julio Fried-
Supporting Information).
mann, Hassan Hassanzadeh, Runan Nygaard and Mehran
The costs of accelerating dissolution arise from the cost Pooladi-Darvish.
of energy required for brine pumping and the capital costs
of the pumps and any additional wells. Considering the base
case described above (Figures 2 and 4), the additional well Supporting Information Available
requirements would include three brine injectors and the Detailed description of reservoir geometry, wells placement,
horizontal segment of the injection well which could numerical discretization, and different reservoir anisotropy
otherwise have a simple vertical completion. The current and inhomogeneity and a video file of simulation results
cost for the required drilling and completing in the Alberta animation. This information is available free of charge via
basin would be of the order of $10 million. (All figures in the Internet at http://pubs.acs.org.
current U.S. dollars. It should be noted that drilling costs are
at historic highs and that such costs are strongly site-specific
(23).) The capital cost of the required pumps and associated
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