Energy 239 (2022) 122233

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Energy
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Fines migration and mineral reactions as a mechanism for CO2

residual trapping during CO2 sequestration
Jiachao Ge, Xiaozhou Zhang, Furqan Le-Hussain*
School of Minerals and Energy Resources Engineering, University of New South Wales, Sydney, NSW, 2052, Australia

a r t i c l e i n f o a b s t r a c t

Article history: This study investigates fines migration and mineral reactions as a mechanism for CO2 residual trapping.
Received 1 August 2021 We perform imbibition experiments using a sintered glass core and seven Berea sandstone cores. The
Received in revised form cores receive four injection stages: water, CO2-saturated water, water-saturated CO2, and finally water or
27 September 2021
CO2-saturated water. During the second injection stage, the quantity of CO2-saturated water is altered to
Accepted 29 September 2021
induce various degrees of fines migration and mineral reactions. These effects are found to yield residual
Available online 1 October 2021
CO2 saturations of 16%, 22% and 23% for zero, 25 and 50 pore volumes of CO2-saturated water injection,
respectively. These percentages are 6e7% greater than if neither fines migration nor mineral reactions
Keywords:
Fines migration
were present. This is attributed to pore plugging caused by fines migration and mineral reactions,
Mineral reactions impeding the imbibing water from displacing CO2 in the plugged pores. In addition, CO2-saturated water
CO2 residual trapping imbibition is found to increase residual CO2 saturation by 26e30% over that resulting from water
Water imbibition imbibition. This is attributed to the CO2 dissolution effect during water imbibition. We therefore
CO2 dissolution conclude that fines migration and mineral reactions is a CO2 residual trapping mechanism during CO2
sequestration.
© 2021 Elsevier Ltd. All rights reserved.

1. Introduction
CO2 injection in subsurface aquifers and oil reservoirs is a po-
tential way to reduce greenhouse gas emissions [1e5]. Four major
trapping mechanisms to secure the sequestration of injected CO2
have been recognised: structural trapping, residual trapping, sol-
ubility trapping, and mineral trapping [6e8]. Structural trapping is
where the upward motion of CO2 is impeded by a low-permeability
caprock. Although it provides immediate and relatively secure
barriers to the migration of CO2 to upper formations, structural
trapping depends on the integrity of the caprock [9e11]. Addi-
tionally, the injected CO2 can be geochemically immobilised either
by dissolving it into the formation water (solubility trapping) or by
forming carbonate minerals through CO2-water-rock reactions
(mineral trapping) [12]. Residual trapping occurs when formation
water imbibes back to the trailing edge of a CO2 plume. The injected
CO2 becomes disconnected by the water displacement and there-
fore trapped in the form of isolated blobs [13,14]. Unlike structural
trapping, residual trapping does not rely on the integrity of the
* Corresponding author.
E-mail address: furqan.hussain@unsw.edu.au (F. Le-Hussain).
caprock [15]. In fact, the isolated CO2 blobs due to residual trapping
have less buoyancy, which reduces upward migration and therefore
the risk of leakage [16]. Residual trapping is therefore considered to
enhance storage security [7,15]. This paper focusses on residual
trapping only.
Previous studies have run core flooding experiments in the
laboratory in an attempt to either reveal mechanisms of CO2 re-
sidual trapping or optimise CO2 residual trapping efficiency. Core
flooding experiments on CO2 residual trapping generally start with
a core fully saturated with water. CO2 is then injected to achieve
initial CO2 saturation ( SCO2 ; i ). This CO2 injection is a process of
drainage, where CO2 is acting as the non-wetting phase to displace
water as the wetting phase. A drainage stage of an experimental run
involving CO2 injection falls into two types. For steady-state
drainage, CO2 and water are injected simultaneously with
increasing fractional flow of CO2 [17e22]. For unsteady-state
drainage, CO2-saturated water is injected before water-saturated
CO2 injection [18,23e32]. CO2-saturated water and water-
saturated CO2 are prepared by equilibrating CO2 and water prior
to injection [26,29]. Once SCO2 ; i is established by CO2 drainage,
water is injected to displace CO2 in the core, so as to achieve re-
sidual CO2 saturation ( SCO2 ; r ). This water injection is an imbibition
process, because water is acting as the wetting phase to displace

https://doi.org/10.1016/j.energy.2021.122233
0360-5442/© 2021 Elsevier Ltd. All rights reserved.
J. Ge, X. Zhang and F. Le-Hussain Energy 239 (2022) 122233

CO2 as the non-wetting phase. 2. Materials and methods

Previous studies have determined that residual trapping can be
affected by intrinsic rock properties including rock type [20,31], 2.1. Fluids
pore network geometry [11,33,34], and pore aspect ratio [35]; by
fluid-fluid interactions including interfacial tension [36] and hys- Ultrapure filtered water was used. To prepare CO2-saturated
teresis [37,38]; or by rock-fluid interactions including wettability water and water-saturated CO2, CO2 and water were equilibrated in
[39,40]. In addition, it has been shown that SCO2 ; r is dependent on an accumulator at experimental conditions (50
C, 10 MPa). Table 1
SCO2 ; i established after CO2 drainage. However, capillary pressure presents the fluid properties at those conditions.
has been the only mechanism of residual trapping found by these
studies.
2.2. Rocks and experimental runs
To our knowledge, no studies have examined the effect of fines
migration and mineral reactions on CO2 residual trapping. During
One sintered glass core (Borosilicate Glass Filter Cylinder,
CO2 sequestration, the injected CO2 can dissolve in the formation
designated G) and seven Berea sandstone cores (designated B1, B2,
water, creating CO2-saturated water. The CO2-saturated water has a
B3, B4, B5, B6, B7) were used. The Berea cores were drilled from the
pH of 3e4, which can dissolve intergranular cements and dislodge
same sandstone block, to maximise similar characteristics. Each
fines [41,42]. The dislodged fines can migrate with the following
core had diameter 2.56 ± 0.02 cm and length 14.2 ± 0.2 cm. Porosity
CO2-water interface and might consequently plug pores [43e46].
was measured to be 0.44 for the glass core, and 0.18 ± 0.02 for Berea
However, none of the fines migration and mineral reaction studies
cores. Table 2 presents the experimental runs (designated by
[28,41,47e52] performed imbibition experiments.
Experiment ID).
Most imbibition studies [17e21,24,25,31,32] injected CO2-satu-
The experimental runs were designed to provide the following
rated water during imbibition to avoid CO2 dissolution in water.
information:
Fewer studies [29,53e55] used water during imbibition. The effect
of imbibition water type on CO2 residual trapping needs to be
1. Exp 5, 7, and 9 were performed to check reproducibility of Exp 4,
examined because imbibition can occur at the tail of a CO2 plume,
6, and 8, respectively.
where water can be un- or under-saturated [53,54]. Berg, Oedai
2. Exp 1 and 2 performed on the glass core were to determine
[29] injected water during imbibition and observed significant CO2
whether CO2 residual trapping would be affected by the injec-
dissolution. CO2 dissolution in the injected water led to reduction in
tion of CO2-saturated water during stage 2. Exp 4, 6, and 8 were
both pressure difference across the core and CO2 saturation in the
analogous for Berea cores. Othman, Naufaliansyah [41,61] found
core. However, the study did not investigate the differences be-
that the injection of CO2-saturated water into Berea cores
tween water imbibition and CO2-saturated water imbibition.
stimulated mineral reactions and created a significant concen-
Chang, Zhou [53] concluded that water imbibition mobilised free-
tration of fines. Ge, Zhang [62] showed that omitting CO2-
phase CO2, resulting in a lower residual CO2 saturation than that
saturated water injection minimised fines migration and min-
from CO2-saturated water imbibition. However, they did not
eral reactions and had negligible effect on CO2 dissolution in
compare pressure difference during imbibition by water versus
water.
CO2-saturated water.
3. Exp 1 and 3 performed on the glass core would show whether
To our knowledge, this is the first study to investigate fines
CO2 residual trapping was affected when water or CO2-saturated
migration and mineral reactions as a mechanism for CO2 residual
water was used for imbibition. Exp 4 and 10 were analogous for
trapping. The rest of the paper is organised as follows. Section 2
Berea cores.
presents materials and methods. Section 3 presents results. Sec-
tion 4 discusses our results. Section 5 states the conclusion.
An additional Berea core was drilled from the same block and

Table 1
Fluid properties at 50
C, 10 MPa.

Water [56] CO2-saturated Water [57,58] Water-saturated CO2 [59,60]

Viscosity (cp) Density (g/cm3) Viscosity (cp) Density (g/cm3) CO2 Solubility (mol/kg) Viscosity (cp) Density (g/cm3)

0.55 1.02 0.57 1.03 1.155 0.0293 0.4048

Table 2
Experimental runs.

Experiment ID Core Type Core Label Absolute Permeability (md) Pore Volumes Injected (PVI) of CO2-saturated Water during Stage 2 Imbibition Water Type

Exp 1 Glass G 619 0 Water

Exp 2 8 Water
Exp 3 0 CO2-saturated water
Exp 4 Berea sandstone B1 21 0 Water
Exp 5 B2 31 0 Water
Exp 6 B3 25 25 Water
Exp 7 B4 25 25 Water
Exp 8 B5 29 50 Water
Exp 9 B6 23 50 Water
Exp 10 B7 32 0 CO2-saturated water

2
J. Ge, X. Zhang and F. Le-Hussain Energy 239 (2022) 122233

Table 3
XRD results for Berea sandstone.

Compound Name Mineral Chemical Formula Quantity [%

Name wt]

Silicon Oxide Quartz SiO2 84.40 (±1.5)

Aluminium Silicate Hydroxide Kaolinite -1A Al2(Si2O5) (OH)4 6.20 (±1.0)
Potassium Aluminium Silicate Microcline Al0.99K0.94Na0.06O8Si3.01 3.8 (±0.5)
Calcium Magnesium Dicarbonate Dolomite CaMg(CO3)2 2.6 (±0.9)
Potassium Aluminium Silicate Muscovite Al3H2KO12Si3[(K0.959Ba0.012Na0.029) (Al1.826 Ti0.033 Fe0.102 Cr0.108 Mg0.11 Mn0.0009) ((Si3.135 Al0.865)O10) 1.90 (±0.3)
Hydroxide -2M1 (O0.502F0.041Cl0.001(OH)1.456)]
Iron Carbonate Siderite FeCO3 1.00 (±0.8)

was subjected to X-Ray Diffraction (XRD) analysis to determine its
mineral composition, as presented in Table 3. Berea core was found
to contain mostly quartz. Intergranular cement in Berea sandstone
is composed of dolomite, siderite, and silicates [63,64].
2.3. Apparatus
Fig. 1 shows a schematic of the experimental setup. Two
continuous-flow ISCO 260D pumps were used: one for CO2 injec-
tion and one for water injection. To inject CO2-saturated water and
water-saturated CO2 into the core, an accumulator was used to
equilibrate the fluids. The core was placed in a coreholder, which in
turn was mounted in a rotational stage. Use of the rotational stage
allows both horizontal and vertical injections. The confining pres-
sure was kept constant at 13 MPa. The back pressure was set at
10 MPa by a backpressure regulator. A high-precision (±0.03 kPa)
pressure transducer measured the pressure difference across the
core. A two-phase acoustic separator recorded the volumes of fluid
produced. An oven maintained a temperature of 50
C.
2.4. Experimental procedure
Prior to each experimental run, the core was fully saturated with
water. Two types of flooding were performed: three-stage flooding
in Exp 1, 3, 4, 5, and 10, and four-stage flooding in Exp 2, 6, 7, 8, and
9. For four-stage flooding, the injection stages are presented below.
Stage 1 and stage 2 were executed with the coreholder horizontal.
In three-stage flooding, stage 2 was omitted.
Stage 1. Inject 20 PVI of water into the core.
Stage 2. Inject CO2-saturated water into the core. To examine the
effect of fines migration and mineral reactions on CO2 residual
trapping, vary the PVI of CO2-saturated water among experimental
runs according to Table 2.
Stage 3. Rotate the coreholder to vertical by adjusting the rota-
tional stage. Inject water-saturated CO2 into the core from the top.
For Berea cores, inject 20 PVI of water-saturated CO2. For the glass

Fig. 1. Schematic of the experimental setup.

3
J. Ge, X. Zhang and F. Le-Hussain
core, inject 7 PVI of water-saturated CO2. Injection of water-
saturated CO2 avoids mass transfer and therefore the drying out
effect [29].
Use the amount of water produced during this stage to calculate
CO2 saturation at the beginning of stage 4. We refer to this satu-
ration as the initial CO2 saturation ( SCO2 ; i ), given by
Vw
SCO2 ; i ¼ ; (1)
Vp
where Vw is volume of water produced during stage 3, and Vp is
pore volume of the core.
Stage 4. Rotate the coreholder by 180
. Inject water (Exp 1, 2, 4,
5, 6, 7, 8, and 9) or CO2-saturated water (Exp 3 and 10) into the core
from the bottom. Continue the injection until CO2 production is
below the detection threshold. Because our accumulator was small,
CO2-saturated water imbibition was not performed in the experi-
ments involving four-stage flooding.
Stages 1, 2, and 3 involved a constant injection rate of 2.5 cc/min
at 50
C and 10 MPa. In stage 4, the injection rate of water or CO2-
saturated water was 1.25 cc/min. Stage 3 represents drainage,
whereas stage 4 represents imbibition. The relation of the injection
stages with real field-scale flow will be explained in the Discussion
section. Pressure difference across the core was measured during
each stage. For Berea cores, the measured pressure difference
during stage 4 was normalised based on the stage 1 pressure dif-
ference measured during Exp 4. Normalised pressure difference
( DPn ) is calculated as
DPm
DPn ¼  DPs1; Exp 4 ; (2)
DPs1
where DPm is the measured pressure difference across the core,
DPs1 is the measured pressure difference during stage 1, and
DPs1; Exp 4 is the measured pressure difference during stage 1 in Exp
4. Normalising the pressure difference allows meaningful com-
parison of experiments involving Berea cores having different
permeabilities.
CO2 produced during stage 4 was reported in pore volumes (PV).
PV of CO2 produced ( PVPCO2 ) is given by
Vg
PVPCO2 ¼ ; (3)
Vp
where Vg is volume of CO2 produced during imbibition (stage 4).
Average CO2 saturation ( SCO2 ) during stage 4 is therefore
calculated as
SCO2 ¼ SCO2 ; i  PVPCO2 : (4)
The ultimate SCO2 at the end of stage 4 is assumed to be the
residual CO2 saturation ( SCO2 ; r ).
Following Exp 4 and 8, Itrax X-ray Fluorescence (Itrax-XRF)
scanning was performed on the injection and production surfaces
of Berea cores to collect elemental profiles. The Itrax-XRF scanner
was programmed to take a reading in precise steps of 200 mm along
a surface. Details of the technique can be found in Kelloway, Ward
[65]. The obtained elemental intensity can provide insights on any
changes in mineralogy due to fines migration and mineral
reactions.
After Exp 8, Scanning Electron Microscopy (SEM) images were
taken of the production surface of the Berea core. Energy-dispersive
X-ray Spectroscopy (EDS) was run to identify minerals present in
the SEM images.
During Exp 2, 4, and 8, samples of water produced during stage 3
4
Energy 239 (2022) 122233
were collected for Inductively Coupled Plasma Optical Emission
Spectrometry (ICP-OES) analysis [66,67].
3. Results
3.1. Reproducibility check
Fig. 2 presents pressure difference and PV of CO2 produced
during imbibition in Exp 4 through 9. For each pair of experimental
runs under the same conditions, the differences in measurements
for the two runs are small enough to be attributable solely to
experimental error, indicating that the experiments in this study
are reproducible. Hence, further analysis will omit Exp 5, 7, and 9.
3.2. Effect of CO2-saturated water injection during stage 2 on CO2
residual trapping
Fig. 3 presents the effect of CO2-saturated water injected during
stage 2 into the glass core on pressure difference, PV of CO2 pro-
duced, and initial and residual CO2 saturation. The quantity of CO2-
saturated water injected during stage 2 did not affect pressure
difference (Fig. 3a), PV of CO2 produced (Fig. 3b), initial CO2 satu-
ration (Fig. 3c), or residual CO2 saturation (Fig. 3d). These findings
are consistent with the expectation of neither fines migration nor
mineral reactions in the glass core.
Fig. 3a presents the pressure difference during water imbibition
in the glass core. Because the water injection rate is constant,
pressure difference (DP) is inversely proportional to the total
mobility (M), given by [68]
ðL
qw 1
DP ¼ dx ; (5)
kab A M
0
where qw is the water injection rate, kab is the absolute perme-
ability of the core, A is the cross-sectional area of the core, L is the
length of the core, and M can be calculated as the sum of water and
CO2 mobilities, given by [68,69]
krCO2 krw
M¼ þ ; (6)
mCO2 mw
where krCO2 is CO2 relative permeability, mCO2 is CO2 viscosity, krw
is water relative permeability, and mw is water viscosity.
Before breakthrough, total mobility decreased as the injection
front reached the production surface of the core. This is because the
increase in water relative permeability was slower than the
decrease in CO2 relative permeability, yielding an increasing trend
of pressure difference. However, after breakthrough, due to
increased water saturation, water relative permeability increased
and therefore total mobility increased, yielding a decreasing pres-
sure difference trend.
Fig. 3b presents PV of CO2 produced. Before breakthrough, PV of
CO2 produced was equal to PV of water injected. After break-
through, rate of CO2 production decreased significantly.
Fig. 3ced presents initial and residual CO2 saturation, respec-
tively. Both saturation values for Exp 2 are 1% less than those for
Exp 1. However, the differences are within experimental error.
Fig. 4 presents the effect of the CO2-saturated water injected
during stage 2 into the Berea cores on pressure difference, PV of CO2
produced, and initial and residual CO2 saturation.
CO2-saturated water injection during stage 2 showed no effect
on the pressure difference or PV of CO2 produced during imbibition.
Endpoint water relative permeability (krw e ) can be calculated
J. Ge, X. Zhang and F. Le-Hussain Energy 239 (2022) 122233

Fig. 2. Comparisons between runs having identical conditions within Exp 4 through 9, of pressure difference and PV of CO2 produced during stage 4, as a reproducibility check.

5
J. Ge, X. Zhang and F. Le-Hussain
Fig. 3. Comparisons of (a) pressure difference, (b) PV of CO2 produced, (c) initial CO2 saturation, and (d) residual CO2 saturation during water imbibition for Exp 1 and 2 on the glass
core.
using the ultimate pressure difference ( DPe ) during imbibition,
given by [68]
qw mw L
krw e ¼ : (7a)
kab ADPe
The calculated krw e was 0.82 ± 0.02 for all experimental runs
performed on Berea cores. Hence, fines migration and mineral re-
actions did not seem to affect water relative permeability, meaning
that water flow was independent of fines migration and mineral
reactions.
Initial CO2 saturation was found to be sensitive to the quantity of
CO2-saturated water injected during stage 2 (Fig. 4c). With 25 PVI
and 50 PVI of CO2-saturated water, initial CO2 saturation was 4% and
7% higher than that without CO2-saturated water injection,
respectively. This can be explained by fines migration and mineral
reactions. Ge et al. [62] established that the injection of CO2-satu-
rated water into Berea cores can dissolve minerals occurring in
intergranular cement, which can dislodge fines [41]. The dislodged
fines can migrate with the subsequently injected water-saturated
CO2 along the flow direction and consequently plug pores. Fig. 5a
6
Energy 239 (2022) 122233
illustrates a pore being plugged by the dislodged fines. Due to pore
plugging, further injected water-saturated CO2 is diverted to pre-
viously unswept pores [9,62,70], yielding higher initial CO2
saturation.
Because PV of CO2 produced is independent of CO2-saturated
water injection, residual CO2 saturation changed only because of
different initial CO2 saturation. As shown in Fig. 4d, with 25 PVI and
50 PVI of CO2-saturated water, residual CO2 saturation was 6% and
7% higher than that without CO2-saturated water injection,
respectively. Fig. 5b illustrates imbibition after pore plugging has
been brought about by fines migration and mineral reactions. The
injected water can displace CO2 only in connected pores, leaving
the CO2 in disconnected pores residually trapped.
Fines migration and mineral reactions were observed only in
Berea cores with CO2-saturated water injection. This was deter-
mined using the Itrax-XRF, which found differences in element
intensity between the injection and production surfaces only when
CO2-saturated water was injected. Fig. 6 presents the intensity of
aluminium (Al) and potassium (K) on the injection and production
surfaces of the Berea cores.
J. Ge, X. Zhang and F. Le-Hussain
Fig. 4. Comparisons of (a) pressure difference, (b) PV of CO2 produced, (c) initial CO2 saturation, and (d) residual CO2 saturation during water imbibition for Exp 4, 6, and 8 on Berea
cores.
Without CO2-saturated water injection, the average intensity of
Al on the production surface was only 8% higher than that on the
injection surface (Fig. 6a). However, when 50 PVI of CO2-saturated
water was injected, the average intensity of Al on the production
surface was 33% higher than that on the injection surface (Fig. 6c).
Without CO2-saturated water injection, the average intensity of
K on the production surface was only 5% higher than that on the
injection surface (Fig. 6b). However, when 50 PVI of CO2-saturated
water was injected, the average intensity of K on the production
surface was 24% higher than that on the injection surface (Fig. 6d).
Al and K were the only chemical elements whose intensity was
measurably different between the injection and production sur-
faces. Al presents in kaolinite, microcline, and muscovite, and K
presents in microcline and muscovite minerals (Table 3). The dif-
ferences in Al and K intensity between injection and production
surfaces indicate that kaolinite, microcline, or muscovite are dis-
placed toward the production surface, due to fines migration or
mineral reactions.
7
Energy 239 (2022) 122233
Fig. 7 presents an SEM image of the production surface of the
Berea core after Exp 8. EDS analysis shows the presence of quartz,
kaolinite, and muscovite. The direct observation of these minerals
in the production surface matched previous studies [28,41,71e74].
Xie, Saeedi [28] found that kaolinite fines detachment and migra-
tion can occur during CO2-water displacement. In addition, Oth-
man, Naufaliansyah [41] observed quartz and muscovite fines
migration during water-saturated CO2 injection into Berea cores.
Further evidence of mineral reactions was obtained by ICP-OES
analysis. Fig. 8 presents the ICP-OES results of produced water for
Exp 2, 4, and 8.
The ICP-OES results show no traces of Ca, Fe, K, or Mg in water
produced by Exp 2. This is expected because there are no reactive
minerals or fines in the glass core.
Production of cations was observed in Berea cores only when
CO2-saturated water was injected during stage 2. Cation production
of Ca, Fe, K, and Mg suggests reactions of dolomite, siderite, and
other cement constituents [62]. This further establishes the
J. Ge, X. Zhang and F. Le-Hussain Energy 239 (2022) 122233

Fig. 5. Schematic of the proposed mechanism of CO2 residual trapping by fines migration and mineral reactions. (a) During drainage, fines migrate at the CO2-water interface by
interfacial force (top left figure). The fines then cause pore plugging (top right figure). If fines migration does not occur (bottom figures), the pore will not be plugged. (b) During
imbibition, water enters the pore throat (left figure). If fines migration occurs (top right figure), water cannot displace CO2 in the plugged pore, leading to more CO2 residual
trapping. If fines migration does not occur (bottom right figure), water displaces CO2 in the pore freely, leading to a small quantity of CO2 being trapped by capillary force.

occurrence of fines migration and mineral reactions due to CO2-
saturated water injection.
3.3. Effect of water and CO2-saturated water imbibition on CO2
residual trapping
Fig. 9 presents the effect of water and CO2-saturated water
imbibition on pressure difference, PV of CO2 produced, and average
CO2 saturation.
Water imbibition led to a later breakthrough by 0.27 PVI for the
glass core and 0.18 PVI for Berea cores, respectively (Fig. 9a and b),
than did CO2-saturated water imbibition. The later breakthrough
during water imbibition might indicate dissolution behind the
injected waterfront. For both water and CO2-saturated water
imbibition, residual CO2 exists behind the waterfront. However, for
water imbibition, some of the residual CO2 was dissolved in the
further injected water; therefore, more of the injected water would
occupy pore space behind the waterfront than in CO2-saturated
water imbibition. This in turn would reduce the speed of the
waterfront, which explains later breakthrough in water imbibition.
Berg, Oedai [29] imaged CO2 saturation using micro-CT, finding
rapid dissolution of CO2 during water imbibition.
For both the glass core and Berea cores, post-breakthrough
pressure difference during water imbibition reduced gradually,
whereas it remained flat during CO2-saturated water imbibition
(Fig. 9a and b). For the glass core, post-breakthrough pressure dif-
ference reduced from 8.8 to 6.3 kPa during water imbibition,
whereas it remained unchanged at 7.7 kPa during CO2-saturated
water imbibition. For Berea cores, post-breakthrough pressure
difference reduced from 450 to 118 kPa during water imbibition,
whereas it slightly reduced from 367 to 353 kPa during CO2-satu-
rated water imbibition. The observed reduction in post-
breakthrough pressure difference during water imbibition can
also be explained by dissolution. As residual CO2 continues to be
dissolved during water imbibition, water saturation and therefore
total mobility increase, yielding a decreasing pressure difference.
Increased total mobility due to CO2 dissolution has been previously
reported [18,53].
Post-breakthrough dissolution of CO2 also led to an increase in
PV of CO2 produced during water imbibition. CO2-saturated water

8
J. Ge, X. Zhang and F. Le-Hussain
Fig. 6. Intensity of Al and K on the injection and production surfaces after experimental runs. Solid lines signify production surfaces, and dotted lines signify injection surfaces.
Fig. 7. SEM image of the production surface of the Berea core after Exp 8. Arrows
indicate where EDS revealed presence of (a) quartz, (b) kaolinite, and (c) muscovite.
imbibition yielded negligible CO2 produced after breakthrough
(Fig. 9c and d), which is typical during water imbibition in strongly
water-wet rocks [75]. Consequently, for the glass core, post-
breakthrough average CO2 saturation reduced from 9% to 4% dur-
ing water imbibition, whereas it reduced slightly from 37% to 34%
during CO2-saturated water imbibition (Fig. 9e). For Berea cores,
post-breakthrough average CO2 saturation reduced from 22% to 16%
9
Energy 239 (2022) 122233
Fig. 8. ICP-OES analysis of produced water from Exp 2, 4, and 8.
during water imbibition, whereas it remained constant at 42%
during CO2-saturated water imbibition (Fig. 9f).
Fig. 9e and f presents average CO2 saturation during water and
CO2-saturated water imbibition. The initial CO2 saturations for
water and CO2-saturated water imbibition are the same. This is
expected because stage 2 (CO2-saturated water injection) was
omitted in these experimental runs. Because water imbibition
produced more CO2 than did CO2-saturated water imbibition,
J. Ge, X. Zhang and F. Le-Hussain Energy 239 (2022) 122233

Fig. 9. Comparisons of pressure difference, PV of CO2 produced, and average CO2 saturation during water imbibition and CO2-saturated water imbibition.

10
J. Ge, X. Zhang and F. Le-Hussain
residual CO2 saturation for the glass core was 4% after water
imbibition and 34% after CO2-saturated water imbibition, and for
Berea cores was 16% after water imbibition and 42% after CO2-
saturated water imbibition.
For the glass core, the difference in residual CO2 saturation be-
tween water and CO2-saturated water imbibition was due to the
dissolution effect. For Berea core, fines migration and mineral re-
actions might also contribute to the difference. Although stage 2
(CO2-saturated water injection) was omitted in these experimental
runs, CO2-saturated water imbibition during Exp 10 into the Berea
core could have dissolve intergranular cements resulting in fines
migration. However, Othman, Yu [48] and Zhang, Ge [43] suggested
that fines generated during CO2-saturated water injection migrate
with the CO2-water interface. Therefore, we assume that negligible
fines migration occurred, as there was no CO2-water interface to
mobilise the fines after CO2-saturated water imbibition. In addition,
the differences between water and CO2-saturated water imbibition
were of similar magnitude in Berea and glass cores. Therefore, the
observed differences presented in Fig. 9 can be mainly attributed to
the dissolution effect during water imbibition rather than to fines
migration and mineral reactions.
To analyse whether capillary forces can differ during the two
types of imbibition, we use the ratio between viscous and capillary
forces, which has been designated [76] Capillary number (Nc ),
given by
vm
Nc ¼ ; (7b)
scosq
where v is the displacing fluid velocity (m/s), m is the displacing
fluid viscosity (Pa.s), s is the interfacial tension (IFT) between dis-
placing and displaced fluids (N/m), and q is the contact angle
Fig. 10. Simulation of a water bearing formation showing the CO2 plume and concentration of dissolved CO2 in water at (a) 30 years of CO2 injection, and (b) 10 years after CO2
injection stopped. The region between boundaries of the CO2 plume at the end of injection and at 10 years after injection stopped represents the residual CO2 saturation.
11
Energy 239 (2022) 122233
(radians). Capillary forces are dependent on IFT and contact angle.
Previous studies [77e79] observed IFT reduction due to CO2
dissolution in water. Under the same experimental conditions as
we used, Li, Boek [77] measured IFT of 35 mN/m between CO2 and
water and 33 mN/m between CO2 and CO2-saturated water. Kaveh,
Rudolph [80] measured a contact angle increase from 25
between
CO2 and water, to 55
between CO2 and CO2-saturated water at
45
C, 10.2 MPa, due to CO2 dissolution in water.
Using the IFT and contact angle values above, the capillary
number is 7  107 for water imbibition, and 1.2  106 for CO2-
saturated water imbibition. Both values are of the same order of
magnitude and therefore do not represent significant change in
flow regime [75,81].
4. Discussion
To examine how the above experimental findings might be
adapted to field-scale CO2 sequestration, we used a simulation
model presented by Hussain, Michael [82]. Simulation run included
CO2 injection into a 100 m-thick water-bearing rock formation for
30 years at 1 Mt/year, followed by a further 70 years without any
injection. Details of the model can be found in the Appendix.
Fig. 10a presents the location of the CO2 plume and the con-
centration of CO2 dissolved in water after 30 years of injection.
Some of the injected CO2 got dissolved in water. The water near the
CO2 plume became fully saturated. Therefore, as the injection
continued, water was displaced by CO2-saturated water followed
by injected CO2. This corresponds to injection stages 1, 2, and 3 in
this study. CO2-saturated water led to mineral reactions and fines
generation. The following CO2-water interface displaced CO2-
saturated water away from the injection well, exposing more of the
J. Ge, X. Zhang and F. Le-Hussain
rock formation to CO2-saturated water. More mineral reactions and
fines generation would occur if the exposure time to CO2-saturated
water is longer. PVI in stage 2 of our experimental runs represents
the exposure time to CO2-saturated water. The CO2-water interface
can mobilise the generated fines, which can plug pores. Therefore,
further injected CO2 would be diverted to other pores that were
previously not swept by CO2, causing the injected CO2 to have
better sweep efficiency.
Fig. 10b presents the CO2 plume locations at the end of CO2 in-
jection and 10 years after the injection was stopped. As the injec-
tion was stopped, CO2 continued to migrate upward due to
buoyancy, which caused water to imbibe into the pores vacated by
CO2. This water imbibition at the edges of the CO2 plume corre-
sponds to stage 4 in this study. The water-imbibed region holds
residual CO2 saturation. In the absence of fines migration and
mineral reactions, the residual CO2 saturation is controlled only by
capillary forces. However, if fines migration and mineral reactions
occur, the imbibing water cannot flow through the plugged pores.
Therefore, these pores will retain more CO2 than would unplugged
pores (see Fig. 5 for schematic and Fig. 4d for experimental
observation).
Fig. 4d show an additional residual CO2 saturation of 6e7%, due
to fines migration and mineral reactions. Such increase in residual
CO2 saturation is significant considering that the field-scale
CO2CRC Otway experiment (Stage 2B) reported residual CO2 satu-
ration of 18%e23% [83]. Furthermore, the increase in residual CO2
saturation reduces the amount of free-phase CO2 that may other-
wise be in contact with the caprock and therefore improves storage
security [84].
The imbibing water near the edges of a CO2 plume can be
partially or fully saturated. Previous studies [54,85] also found that
dissolved CO2 at the plume edges can be in contact with unsatu-
rated water. Therefore, we performed both water and CO2-satu-
rated water imbibition (section 3.3). However, to complete the
picture, experiments should be performed where CO2-saturated
water is used in stage 2 and again during imbibition in stage 4. Due
to the limited capacity of our accumulator, such experiments were
not performed.
5. Conclusion
In this study, we performed experiments on a sintered glass core
and Berea sandstone cores to examine the effect of fines migration
and mineral reactions on CO2 residual trapping, as well as to
differentiate between water imbibition and CO2-saturated water
imbibition.
Our observations lead to the following conclusions:
 Fines migration and mineral reactions can lead to higher re-
sidual CO2 saturation.
For Berea cores, residual CO2 saturation was dependent on the
quantity of CO2-saturated water injection, which is known to
cause fines migration and mineral reactions. Following 25 and
50 pore volumes of CO2-saturated water injection, residual CO2
saturation was 22% and 23%, respectively, compared to 16% for
where no CO2-saturated water was injected.
For the glass core, CO2-saturated water injection had negligible
effect on CO2 residual trapping. This is attributed to the absence
of fines migration and mineral reactions in the glass core.
12
Energy 239 (2022) 122233
In addition, fines migration and mineral reactions did not affect
pressure difference or endpoint water relative permeability
during water imbibition.
 For both the glass core and Berea cores, CO2 residual trapping
presented distinctive differences between water and CO2-satu-
rated water imbibition, due to dissolution during water imbi-
bition. Both water imbibition and CO2-saturated water
imbibition can occur near the edges of CO2 plume during a real
CO2 sequestration project.
Water imbibition led to a later breakthrough by 0.27 PVI for the
glass core and 0.18 PVI for Berea cores, respectively, compared to
that during CO2-saturated water imbibition.
Post-breakthrough pressure difference reduced during water
imbibition but remained fairly constant during CO2-saturated
water imbibition.
Due to the dissolution effect, residual CO2 saturation for the
glass core was 4% after water imbibition versus 34% after CO2-
saturated water imbibition, and for Berea cores was 16% after
water imbibition versus 42% after CO2-saturated water
imbibition.
Due to the limited capacity of our equipment, CO2-saturated
water imbibition was not performed for experimental runs with
CO2-saturated water injection before drainage. Such experi-
ments should be performed to further assess the effect of fines
migration and mineral reactions on CO2 residual trapping.
In conclusion, fines migration and mineral reactions were found
to be a CO2 residual trapping mechanism. The induced residual
trapping contributes to safer storage because it reduces the amount
of free-phase CO2 that may be in contact with the caprock. Addi-
tionally, we observed a dissolution effect during water imbibition
but not during CO2-saturated water imbibition.
Credit author statement
Jiachao Ge: Writing - Original Draft, Methodology, Data Cura-
tion, Investigation, Formal analysis, Visualization Xiaozhou Zhang:
Formal analysis Furqan Le-Hussain: Supervision, Conceptualiza-
tion, Writing- Reviewing and Editing, Methodology, Resources,
Formal analysis.
Declaration of competing interest
The authors declare that they have no known competing
financial interests or personal relationships that could have
appeared to influence the work reported in this paper.
Acknowledgements
The authors acknowledge David H. Levin (Murphy, NC, USA) for
editing the manuscript; and the Mark Wainwright Analytical
Centre, UNSW for providing ICP-OES and SEM-EDS services. Jiachao
Ge thanks UNSW and the China Scholarship Council (CSC) for
providing funding for his PhD studies.
APPENDIX. Field-scale CO2 sequestration simulation
The commercial compositional reservoir simulator Eclipse
300™ was used to model CO2 injection and subsequent water
imbibition in a sequestration formation. Table A1 presents the pa-
rameters of the simulation model.
J. Ge, X. Zhang and F. Le-Hussain
Table A1
Parameters of the simulation model
Number of grid blocks
Grid block size in x-direction (block numbers 1 to 24 and 28 to 51)
Grid block size in x-direction (block numbers 25 and 27)
Grid block size in x-direction (block number 26)
Grid block size in y-direction
Grid block size in z-direction
Top depth
Initial pressure at top depth
The relative permeability of CO2 ( krg ) and water ( krw ) and the
capillary pressure ( Pc ) used in the model were generated using
the following equations:
 3:5
Sw  0:2
krw ¼ ; (A1)
0:6
 
Sg  0:2 2:2
krg ¼ 0:87  ; (A2)
0:6
 3:5 !0:6
Sw  0:2
Pc ¼ 12  1 ; (A3)
0:8
where Sw is the water saturation.
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