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ABSTRACT
Natural gas reservoirs are obvious targets for carbon
sequestration by direct carbon dioxide (CO2)
injection by virtue of their proven record of gas
production and integrity against gas escape. Carbon
sequestration in depleted natural gas reservoirs can be
coupled with enhanced gas production by injecting
CO2 into the reservoir as it is being produced, a
process called Carbon Sequestration with Enhanced
Gas Recovery (CSEGR).
In this process,
supercritical CO2 is injected deep in the reservoir
while methane (CH4) is produced at wells some
distance away. The active injection of CO2 causes
repressurization and CH4 displacement to allow the
control and enhancement of gas recovery relative to
water-drive or depletion-drive reservoir operations.
Carbon dioxide undergoes a large change in density
as CO2 gas passes through the critical pressure at
temperatures near the critical temperature. This
feature makes CO2 a potentially effective cushion gas
for gas storage reservoirs. Thus at the end of the
CSEGR process when the reservoir is filled with
CO2, additional benefit of the reservoir may be
obtained through its operation as a natural gas storage
reservoir. In this paper, we present discussion and
simulation results from TOUGH2/EOS7C of gas
mixture property prediction, gas injection,
repressurization, migration, and mixing processes
that occur in gas reservoirs under active CO2
injection.
INTRODUCTION
Depleted natural gas reservoirs are promising sites
for geologic carbon sequestration by direct carbon
dioxide (CO2) injection. First and foremost, natural
gas reservoirs have a demonstrated integrity against
gas escape shown by their long term containment of
methane (CH4) and capacity estimated at 140 GtC
worldwide (IEA, 1997) and 10 to 25 GtC in the U.S.
alone (Reichle et al., 1999). Second, past production
activity has allowed them to be relatively well
characterized and well understood. Third, there is an
existing infrastructure of wells and pipelines and
associated land use history amenable to an industrial
process such as direct CO2 injection. These positive
-2-
CO2
Solid
100.
73.8
103
P, T path
10.
5.2
1.
0.1
-78.5 -56.4
104
Liquid
critical point
Gas
-20.
102
Depth (m)
1000.
P (bars)
10.
31.0
T (C)
Figure 1. Phase diagram of CO2 showing typical P,
T path assuming hydrostatic pressure and
25 C km-1 geothermal gradient.
Z=
PV
nRT
(1)
Phase Diagram
The phase diagram for CO2 is shown in Figure 1,
along with a typical P, T path assuming hydrostatic
pressure and 25 C km-1 gradients with depth in the
earth. As shown, CO2 will be supercritical (Pcrit =
73.8 bar, Tcrit = 31.0 C (Vargaftik, 1975)) in gas
reservoirs that are typically at depths greater than 1
km and hotter than 35 C. In depleted reservoirs,
pressures can be below hydrostatic and subcritical
conditions may exist. Therefore, the simulation
capability must treat both supercritical and gaseous
states of CO2.
-3-
1
(pure C
H
800
x
x=
x=
=
1.
0. 5
ur
)
O2
eC
Density (kg/m3)
(p
0.7
x=
400
0.6
0.5
0.4
.50
x=0
0.3
T = 40 C
5
x = 0.2
200
ure CH 4)
x = 0.0 (p
100
0
0.80
0.70
x=
300
0.9
0.8
.90
x=0
600
500
CO 2)
.95
x=0
700
ure
1.0 (p
Z value (-)
900
0.2
0.1
20
40
60
80
100
120
140
160
180
0
200
Pressure (bar)
flue gas
power plant
800
compressor
CO2
CH4
T = 40 C
CH4
600
CO2
400
200
0
1 bar
61 bars
101 bars
141 bars
181 bars
7.5 x 10-5
5.0 x 10-5
2.5 x 10-5
CO2
0.8
0.6
0.4
0.2
0.0 x 10-5
Viscosity (Pa s)
Density (kg/m3)
CH4
depleted natural
gas reservoir
-4-
Table 1. Properties of CO2-CH4 gas mixtures and aqueous solubility at 40 and 100 bars, 40 C.
P = 40 bars, T = 40 C
gas phase
aqueous phase
Prediction Source
xgCH4
xgCO2
(kg m-3)
(Pa s)
xlCH4
xlCO2
-5
TOUGH2/EOS7C
0.
1.
85.45
1.70 x 10
0.
1.62 x 10-2
-5
Reference Values
0.
1.
83.79 [1]
1.73 x 10 [1]
0.
1.37 x 10-2 [2]
-5
-4
TOUGH2/EOS7C
0.5
0.5
51.97
1.44 x 10
3.73 x 10
8.07 x 10-3
-5
-4
Reference Values
0.5
0.5
51.33 [1]
1.67 x 10 [1]
3.66 x 10 [3,4,5,6]
6.74 x 10-3 [3,4,5,6]
-5
-4
TOUGH2/EOS7C
1.
0.
26.42
1.21 x 10
7.43 x 10
0.
Reference Values
1.
0.
26.10 [1]
1.23 x 10-5 [1]
7.22 x 10-4 [3,4,5,6]
0.
P = 100 bars, T = 40 C
gas phase
aqueous phase
TOUGH2/EOS7C
0.
1.
566.00
4.35 x 10-5
0.
4.03 x 10-2
-5
Reference Values
0.
1.
631.90[1]
5.04 x 10 [1]
0.
2.19 x 10-2 [2]
-5
-4
TOUGH2/EOS7C
0.5
0.5
155.16
1.81 x 10
9.43 x 10
2.00 x 10-2
Reference Values
0.5
0.5
153.97 [1]
1.94 x 10-5 [1]
7.95 x 10-4 [3,4,5,6]
1.21 x 10-2 [3,4,5,6]
-5
-3
TOUGH2/EOS7C
1.
0.
71.57
1.41 x 10
1.86 x 10
0.
Reference Values
1.
0.
70.03 [1]
1.41 x 10-5 [1]
1.54 x 10-3 [3,4,5,6]
0.
1
NIST, 1992. 2 Wiebe and Gaddy, 1940. 3 Spycher and Reed, 1988. 4 Johnson et al., 1992. 5 Shock et al., 1989.
6
Wagman et al., 1982.
pipeline gas
shale
cushion
gas
sand
sand
CH4
working
gas
CH4
working
gas
sand
cushion
gas
(a)
(b)
shale
CH4 production
5 mi
(8 km)
SIMULATION METHODS
For the simulation of CSEGR and gas storage with
CO2 as a cushion gas, we are using a new module
called TOUGH2/EOS7C.
This module was
developed by extending EOS7R (Oldenburg and
Pruess, 1995; Pruess et al., 1999) by changing one of
the volatile components to CO2, and by changing the
air to CH4. Thus, EOS7C considers five mass
components (water, brine, CO2, gas tracer, CH4) and
heat. Solubility subroutines for CO2 and CH4 were
CO2 Injection
Monitoring Well
CSEGR
We have used TOUGH2/EOS7C to carry out a
number of CSEGR simulation studies over the last
several years (e.g., Oldenburg et al., 2001; Oldenburg
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CH4
Production
(a)
Value
6.4 x 105 m2
(160 acres)
50 m (160 ft)
0.30
1 x 10-12 m2
0.20
Immobile.
Equal to gas
saturation.
1.0 x 10-5 m2 s-1,
1.0 x 10-10 m2 s-1
75 C (167 F)
50 bars (725 psi)
3 kg s-1 (260 t/day)
0.56 kg s-1
(48 t/day)
60 bars (870 psi)
1
0.9
0.8
0.7
0.6
0.5
0.4
0.3
0.2
0.1
0
CO2
Injection
-25
800
-50
800
400
400
Y (m)
CH4
Production
(b)
00
)
(m
injection interval
t = 15 yrs
production interval
110
100
90
80
70
60
50
40
CO2
Injection
0
Z (m)
Property
Quarter five spot size
(21 x 21 gridblocks in X-, Ydir.)
Reservoir thickness
(10 gridblocks in Z-dir.)
Porosity
Permeability (isotropic)
Residual liquid saturation
Relative permeability
Liquid
Gas
Z (m)
XgasCO2
t = 15 yrs
production interval
-25
800
-50
800
400
400
Y (m)
00
)
(m
injection interval
Value
4 km x 1 km (1.5 mi2)
22 m
1 x 200
11
0.30
1.0 x 10-12 m2
Van Genuchten (1980)
0.2, 0.27, 1, 0.01
Sl 0.26 < Slr
1.0 x 10-6, 1.0 x 10-10
40 C (isothermal)
60 bars
73.5 kg s-1
-6-
XCO2
g
150
0.8
0.9
0.7
0.1
0.2
0.3
CH4
140
CO2 Cushion
0.5
0.6
0.1
-15
0.4
Z (m)
-5
-10
0.4
-20
0.7
130
0.80.9
250
500
750
1000
Y (m)
(b)
XCO2
g
0
0.1
CH4
-10
0.4
0.2
-15
0.3
0.8
0.9
0.5
0.6 0.7
CO2 Cushion
0.1
0.3
Z (m)
-5
-20
0
250
500
750
CH4
0.8
-20
0.5
0.9
60
0.1
250
0.7
0.4
0.3
0.2
Z (m)
0.5
-15
500
750
1
11
17
86
173
4
1
16 4 8
1
74
62
11
-20
3
186
86
CH4
-15
12
Z (m)
-5
99
13
CO2 Cushion
186
250
500
750
1000
Y (m)
-3
12
Z (m)
15
CH4
-10
10
17
2 21197
2865 9
7
310
g (kg m )
0
-5
6
2
24
84
-15
129
151
174
197 219
265 7
28
CO2 Cushion
310
-20
0
250
500
750
1000
Y (m)
g (kg m-3)
264
Z (m)
-5
CH4
-10
128
174
-15
264
354
489
21
309
9
CO2 Cushion
-20
0
250
500
579
399
444
534
750
1000
g (kg m-3)
-10
Time (months)
CO2 Cushion
0.8
0.6
0.9
Y (m)
(c)
90
0.6
-10
(b)
100
70
0.3
0.2
-5
(a)
110
80
XCO2
g
CO2 cushion
CH4 cushion
CH4 cushion, 70% injection
120
1000
Y (m)
(c)
Pressure (bars)
(a)
1000
Y (m)
-7-
ACKNOWLEDGMENT
I thank Christine Doughty and Andr Unger (LBNL)
for reviews. Special thanks to George Moridis for
developing the gas properties subroutines used in
TOUGH2/EOS7C. I also thank Karsten Pruess,
Alfredo Battistelli, and Sally Benson for assistance
with this research. This work was supported in part
by the Assistant Secretary for Fossil Energy, Office
of Coal and Power Systems through the National
Energy Technology Laboratory, and by Lawrence
Berkeley National Laboratory under Department of
Energy Contract No. DE-AC03-76SF00098.
REFERENCES
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