Natural Resources Research (Ó 2019)

https://doi.org/10.1007/s11053-019-09553-x

Original Paper

A Study on the Surface Wettability of Clastic Rocks

with Potential Application for CO2 Storage Sites

Bappah Adamu Umar,1 Raoof Gholami,2,8 Arshad Raza,3 William Samuel Downey,4
Mohammad Sarmadivaleh,5 Afroz A. Shah,6 and Prasanta Nayak7

Received 7 February 2019; accepted 28 August 2019

There have been many studies carried out in the past decades attempting to develop
strategies for a safe injection of CO2 into storage sites without leakage and contamination of
valuable resources. Leakage from these storage sites through capillary seals is one of the
long-standing issues, which require a comprehensive assessment prior to CO2 injection.
However, surface wettability, which is one of the major parameters controlling the capillary
pressure of seals, is a poorly understood parameter, changing as a function of temperature,
pressure, surface roughness, etc. The aim of this paper is to provide a deeper insight into the
surface wettability of minerals in rocks, especially sandstone and shales, under subsurface
conditions for a better assessment of the structural integrity in CO2 storage sites. The results
obtained from a series of contact angle measurements under different pressure and tem-
perature conditions indicated that quartz- and feldspar-dominated sandstones are strongly
water wet, while kaolinite-dominated shales have a weakly water to intermediate wet sys-
tem. It is also apparent that the interfacial tension is a function of the pressure and tem-
perature conditions. It appears that the size of pore throats in rocks is the major contributor
to capillary threshold pressure and it must be determined very accurately. It is recommended
that surface wettability and interfacial tension under reservoir conditions are determined a
priori to ensure that the seal integrity analysis is as concise as possible.
KEY WORDS: CO2 storage, Wettability, Interfacial tension, Pore throats, Seal integrity.

INTRODUCTION
1
National Center for Petroleum Research and Development,
Abubakar Tafawa Balewa University, Bauchi, Nigeria. Geological storage of carbon dioxide (CO2) is
2
Department of Petroleum Engineering, Curtin University, Miri,
presently regarded as a key solution to reduce the
Malaysia.
3
Department of Petroleum & Gas Engineering, UET Lahore, amount of greenhouse gases released into the
Lahore, Punjab, Pakistan. atmosphere. The efficiency and long-term security of
4
Department of Applied Geology, Curtin University, Miri, a storage practice, on these occasions, depend on the
Malaysia. ability of selected reservoirs and seal to hold the
5
Department of Petroleum Engineering, Curtin University, Perth,
injected CO2 for thousands of years (Qing et al.
Australia.
6
Department of Geology, Universiti Brunei Darussalam, Gadong, 2013). However, despite successful implementations
Brunei. of the carbon capture and storage (CCS) technology
7
Shell Petroleum Company Ltd, Plaza Shell, Kota Kina- in many countries, the issue of leakage from storage
balu, Sabah, Malaysia. sites has remained unsolved (Miocic et al. 2014;
8
To whom correspondence should be addressed; e-mail:
Wollenweber et al. 2010).
[email protected]

Ó 2019 International Association for Mathematical Geosciences

 B. A. Umar et al.

Faults are discontinuities commonly found in unsaturated conditions where CO2 bubble dimen-
many geological settings where potential storage sions changed with time due to dissolution. Jafari
sites are located. However, although it is assumed and Jung (2018) investigated the variation of contact
that faults are impermeable due to shale gouge or angle on the mica surface at a wide range of pres-
clay smear, many of them are membrane or capillary sures and salinities under unsaturated conditions.
seals (Yielding 2015). As a capillary seal, the maxi- They found a general increase in the contact angle
mum column height of CO2 sustainable by a fault is with time. It seems that the reported contact angles
a function of the interfacial tension (r), the pore vary in different studies, while mica may not even be
throat size (r) of the rocks surrounding the fault and an appropriate proxy for clays when determining
the wettability of the fault surface (Bretan and wettability characteristics.
Yielding 2005; Bretan et al. 2011). Surface wetta- The aim of this paper is to provide a deeper
bility is perhaps the most important parameter in a insight into the surface wettability of minerals in
capillary seal, but it is a poorly understood param- rocks, especially sandstone and shales, for a better
eter due to the heterogeneity of rocks on various assessment of the structural integrity in CO2 storage
scales. There have been several attempts to deter- sites. A series of contact angle and interfacial ten-
mine the surface wettability of quartz- and feldspar- sion measurements were made under different
dominated rocks under the reservoir conditions for pressure, temperature and salinity conditions to see
the evaluation of residual trapping, in order to im- if the results reported so far are trustworthy or that
prove structural trapping in CCS sites (e.g., Broseta further investigations are necessary.
et al. 2012; Mutailipu et al. 2019; Sarmadivaleh et al.
2015). However, limited studies have been carried
out on clays due to their small crystal size. In fact, Capillary Pressure and Surface Wettability
most of these measurements have been on the mica
group rather than clays because of their perceived As mentioned earlier, capillary pressure is a
similar physical and chemical characteristics. For function of surface wettability and plays a major role
instance, Chiquet et al. (2005) reported different in the integrity of membrane seals. Wettability is
wetting regimes for mica including an intermediate defined as the ability of a fluid to wet the rocksÕ
wetting behavior. They measured the contact angles surface in a three-phase system consisting of rock,
under three different brine conditions (0.01, 0.1 and aqueous and non-aqueous phase fluids (e.g., oil or
1 M NaCl) and concluded that the contact angle CO2) (Iglauer et al. 2015).
varies from 0 to 20° for a low-pressure mica. This In petroleum engineering-related discussions,
range, however, becomes 60°–80° when the pressure wettability is often classified into three groups based
is increased to 10 MPa. Chiquet et al. (2007) and on variations in contact angles. This classification
Broseta et al. (2012) measured advancing and can also be applied to brine–CO2–rock systems
receding contact angles as a function of the pressure where CO2 wet is used rather than oil wet in some
and salinity. They pointed out that the advancing definitions. However, the contact angle defining the
contact angles are generally higher (between 35° and wetting and non-wetting phases is expressed differ-
100°) than the receding (between 18° and 70°) but ently in many textbooks. For the purpose of this
did not observe any changes in the measurements study, the definition provided in Table 1 is followed.
with respect to salinity. Mills et al. (2011) stated that There are, however, many parameters including
the contact angle of biotite varies between 35° and pressure, temperature, surface contamination and
40° at a temperature of 313 K and salinity of roughness, which may alter the wettability of sur-
35,000 ppm. Farokhpoor et al. (2013a) did not reach faces (e.g., Ali et al. 2019a, b; Arif et al. 2016; Iglauer
the same conclusion and reported a remarkable et al. 2015). As a result, more studies are required to
lower advancing contact angle for mica, which might ensure that the surface wettability obtained from the
be linked to the surface cleaning procedure em- laboratory measurements can be applied to field
ployed. Wang et al. (2013) reported a low and con- conditions. In the next sections, attempts are made
stant receding contact angle of 20° for magnesium- to evaluate the surface wettability of sandstone and
rich mica. This contact angle, however, increased to shale, the two clastic rocks commonly found in fault
43° at pressure and temperature of 20 MPa and zones.
323 K, respectively. Jafari and Jung (2016) noted the
change in contact angle on the mica surface at
A Study on the Surface Wettability of Clastic Rocks

Table 1. Wettability based on the contact angle for CO2–brine– at the experimental conditions in a high-pressure
mineral system (Iglauer et al. 2015) mixing reactor, following the equilibrium procedure
Wettability Water contact angle (h°) reported by El-Maghraby et al. (2012). Surface
cleaning was carried out using acetone (with a purity
Complete wetting or 0
of 99.9 mol%), while aqueous hydrochloric acid was
spreading of water
Strongly water wet 0–50 used to control the pH of the brine. Deionized water
Weakly water wet 50–70 was used to remove dust or surface fragments from
Intermediate wet 70–110 the substratesÕ surface. This was followed by drying
Weakly CO2 wet 110–130 the samples in an oven at 90 °C for 60 min. Air
Strongly CO2 wet 130–180
plasma was then used for 15 min to erase any or-
Complete non-wetting of water 180
ganic contamination from the substrates. Subse-
quently, ultra-clean N2 was applied to clean
mechanically any remaining water from the surface
MATERIALS AND METHODS to avoid contamination. Degassed (i.e., vacuumed
for 10 h) brine solutions were dispensed onto the
Substrates substrateÕs surface to measure the contact angle
using a high-resolution camera. The temperature of
Three samples including kaolinite-dominated the cell was increased from room temperature to
shale together with sandstones dominated by quartz 35 °C, and CO2 gas was injected at the ambient
and feldspar with the compositions provided in Ta- condition for 10 min, followed by pressurizing the
ble 2 were considered for the purpose of this study. cell with a high-precision syringe pump to 17 MPa.
A series of tests were carried out to determine the The temperature was then increased to 65 °C, and
pore throat size of the samples using the mercury each test was repeated three times to measure the
intrusion porosimeter and gas adsorption methods. advancing and receding contact angles using a 15-
It should be noted that the mercury injection degree-angle surface plate in the system as shown in
porosimeter cannot be used for tight rocks due to Figure 3.
their nanosized pore structure and as such, the gas
(nitrogen) adsorption technique was used to deter-
mine the pore size distribution within the shale Interfacial Tension Measurements
samples. The results obtained from such tests can be
used to determine the capillary pressure provided by The interfacial tension was determined based
each of the samples of rocks during CO2 injection. on the pendant drop method using the same appa-
Figure 1 shows that the used pore throatsÕ sizes of ratus as used to measure the contact angle. In this
samples of the quartz- and feldspar-dominated approach, the cell was heated up and flooded with
sandstones are close to 10 micrometers, while that of CO2 for at least 10 min and the pressure was in-
shale is approximately 0.1 nm. creased from 0.1 to 17 MPa to have supercritical
CO2 in place. To achieve this, the supercritical pump
was heated up to 40 °C and brought to the experi-
Contact Angle Measurements mental pressure of 17 MPa. The reactor in an oil
bath was heated to the experimental conditions,
Contact angle measurements were carried out vacuumed and filled with deaerated brine via the
using the Kruss Drop Shape Analyzer (DSA100 syringe pump. Brine in the reactor was then dis-
HP), schematically shown in Figure 2, at different placed by scCO2 and isolated. By stirring at 200 rpm,
pressure (0–17 MPa) and temperature conditions CO2 and brine were brought to equilibrium inside
(20–65 °C). These ranges of pressure and tempera- the reactor. During this process, the pressure inside
ture were chosen given the fact that the majority of the reactor was stabilized and was monitored using
changes in wettability have been reported to be transducers. In addition, the volume and pressure of
within this range (Al-Yaseri et al. 2016; Farokhpoor the pump were logged to monitor the balance of
et al. 2013b; Sarmadivaleh et al. 2015). CO2 with a scCO2 volume. Equilibrium was achieved after
purity of 99.9% was used together with brine (NaCl 60 min. Deionized water and brine were then slowly
solution with concentrations of 0 to 35 wt%) to released from the needle inside the cell, which
perform the tests. Brine was equilibrated with CO2 formed as a drop at the bottom of the injection
 B. A. Umar et al.

needle. From the shape of the drop captured by the

Illite–smectite
high-resolution camera, the interfacial tension (r)

(%)

5.01
2.21
3.4
was calculated as (Sarmadivaleh et al. 2015):
qg
r¼ ; ð1Þ
ðbKapex Þ2

15.19
Illite
(%)

13.8
6.2
where Kapex is the curvature at the apex point of the
drop, b is the shape parameter (dimensionless), q is
Chlorite

the density of the drop and g is the gravitational

(%)

6.12
5.1
0.7 acceleration.
Kaolinite

32.21

RESULTS
(%)

1.7
0.7
Table 2. Mineral compositions of the sandstone and shale samples used in this study

Quartz-Dominated Sandstone
Biotite
(%)

0.11
2.3

0.8

The contact angles (h) were measured at dif-

ferent pressures (0.1, 5, 10 and 17 MPa) and tem-
peratures (20, 35 and 65 °C) for the samples
Muscovite

described earlier. The results obtained from the

(%)

0.03
1.5

0.5

quartz-dominated sandstone indicated that, as the

salinity increases, the contact angle correspondingly
increases (Fig. 4, left) and the contact angle of brine
Plagioclase

(NaCl solution) is greater than that of the deionized

(%)

0.01
0.01
0.01

water. According to Al-Yaseri et al. (2016), this in-

crease in the contact angle changes with the salt type
(MgCl2, CaCl2 and NaCl) and is linked to the dif-
ferences in the cation charge-to-volume ratio, which
K feldspar

0.16
0.33

leads to an effective shielding. The degree of in-

(%)

45

crease in the contact angle is higher for MgCl2

compared to CaCl2 with NaCl, showing a lower in-
crease than CaCl2.
(weight %)

It was also found that the contact angle of the

Quartz

37.5
85.2

quartz-dominated sandstone increases with increas-

35

ing pressure at different temperature (Fig. 4, right).

This could be due to the increase in CO2 density
under reservoir conditions, which enhances the
Grain density
(g/cm3)

intermolecular interactions between CO2 and

2.55
2.65
2.8

quartz, causing de-wetting of the surface. At the

ambient condition, however, the receding contact
angle of CO2/brine/quartz system was 20 °C, which
is similar to that shown by Al-Yaseri et al. (2016).
Sandstone 2 (feldspar-dominated)
Sandstone 1 (quartz-dominated)
Shale (kaolinite-dominated)

Feldspar-Dominated Sandstone

There have been several studies on the wetta-

bility of feldspars (Farokhpoor et al. 2013b; Wang
et al. 2012) where it was indicated that the variation
Rock type

of the wettability and contact angle for feldspars is

not as complex as that of quartz. In this study, it is
A Study on the Surface Wettability of Clastic Rocks

Sandstone (Quartz Dominated) Sandstone (Feldspar Dominated)

0.9 0.9
Incremental
0.8 0.8 Cumulative

Cumulative Pore Space (farction)

Cumulative Pore Space (farction)

0.7 0.7

0.6 0.6

0.5 0.5

0.4 0.4

0.3 0.3

0.2 0.2

0.1 0.1

0 0
10 -2 10 0 10 2 10 4 10 -2 10 0 10 2 10 4
Pore Throat Radius (Um) Pore Throat Radius (Um)

Shale Sample
0.9
Incremental
0.8 Cumulative
Cumulative Pore Space (farction)

0.7

0.6

0.5

0.4

0.3

0.2

0.1

0
10 -4 10 -2 10 0 10 2
Pore Throat Radius (Nm)
Figure 1. Pore throat size distribution of sandstone and shale samples used in this study.

shown that feldspar-dominated sandstone has a once the pressure increases from 0 to 17 MPa. The
completely water wet system (with the contact angle range of receding angle for the same range of pres-
between 6° and 23°) and can be regarded as an sure was 6° to 14.4°, 9° to 16.7° and 12° to 19.8° at
efficient barrier against the migration of CO2 al- 20 °C, 35 °C and 65 °C, respectively (Fig. 5, right).
though the pore throat size must be carefully eval- These results are consistent with the findings of Ig-
uated. The results obtained also indicated that the lauer et al. (2015), who indicated that the contact
advancing contact angle of feldspar-dominated angle of feldspar is almost independent of pressure
sandstone varies from 8° to 17.8°, 11° to 19.8° and and temperature conditions. On the other hand,
14° to 22.8° at 20 °C, 35 °C and 65 °C, respectively, there were minor changes in the contact angle of the
 B. A. Umar et al.

feldspar with respect to the salinity level, as shown in studies have reported the wettability of kaolinite
Figure 5 (left side), and these are consistent with the (Borysenko et al. 2009; Wang et al. 2012), but none
finding of Farokhpoor et al. (2013a), who empha- have included measurements under different pres-
sized that the contact angle is not very sensitive to sure, temperature and salinity conditions. The re-
changes in the salinity of brine. However, it would sults obtained from this study indicated that the
be wise to consider the ionic strength of brine for an wettability of kaolinite-dominated shale is sensitive
accurate estimation of the capillary pressure. to variations in temperature and pressure conditions.
It would be weakly water wet under ambient con-
ditions and becomes intermediately wet when the
Kaolinite-Dominated Shale pressure is raised to 17 MPa and at a temperature of
65 °C (Fig. 6).
There have been only few attempts so far to Figure 6 shows that the advancing contact angle
measure the wettability of clays with most studies may vary from 64° to 74° at different pressure and
carried out using mica due to its supposed physical temperature conditions, while the receding contact
and chemical similarities to clay minerals. Some angle may change from 63° to 72° as both pressure
and temperature increase. This highlights the fact
that kaolinite-dominated shale may not be an
effective barrier, as generally accepted, against the
migration of CO2 under reservoir conditions. Unlike
quartz and feldspar, the contact angle of CO2/water/
kaolinite decreased by increasing the salinity (Fig. 6,
left side). In fact, the results obtained indicate that
the contact angle created by the deionized water is
Light
Camera higher than that created by the brine drop. This
reduction might be linked to the variation of zeta
CO2 Pump Water Pump
potentials or due to the increase in the ionic
HPHT Cell strength. High negative zeta potentials lead to high
polar surfaces and a better water wettability. How-
ever, the surface wettability did not reach the
Computer strongly water wet condition even under a salinity
level of 36% wt NaCl. This observation, on the
Figure 2. Schematic view of the drop shape analyzer used other hand, could be linked to the fact that clays
for the interfacial tension and contact angle measurements. have active surface charges and NaCl is not the best
agent to inhibit clay–water interactions. In fact, if

Figure 3. Optical images of brine drop on the surface of shale.

A Study on the Surface Wettability of Clastic Rocks

o
Measurements @ 17 MPa and 35 C Quartz Wettability
50 45
Receding (T=20 C)
Receding (T=35 C)
45 40 Advancing (T=20 C)
Advancing (T=35 C)
35 Advancing (T=65 C)
40 Receding (T=65 C)
Contact Angle (Degree)

Contact Angle (Degree)

30
35
25
30
20
25
15

20
10

15 Advancing
5
Receding

10 0
0 5 10 15 20 25 30 35 0 5 10 15
Salinity (wt%) Pressure (MPa)

Figure 4. Advancing and receding contact angles for CO2/water/quartz as a function of salinity (left) and pressure and temperature
(right).

Measurements @ 17 MPa and 35 o C Feldspar Wettability

25 24
Advancing Advancing (T=20 C)
Advancing (T=35 C)
Receding 22 Advancing (T=65 C)
Receding (T=20 C)
20 Receding (T=35 C)
20 Receding (T=65 C)
Contact Angle (Degree)

Contact Angle (Degree)

18

16
15
14

12

10
10

5 6
0 5 10 15 20 25 30 35 0 5 10 15
Salinity (wt%) Pressure (MPa)

Figure 5. Advancing and receding contact angles for CO2/water/feldspar as a function of: salinity (left) and pressure and
temperature (right).

clays crystalline/osmotic swelling cannot be stabi- It should be noted that surface roughness is also
lized by the brine, changing its surface wettability an important parameter in the determination of the
may not be an easy task. contact angle and it may alter the surface wettabil-
ity. Thus, the best practice would be to use a very
 B. A. Umar et al.

Measurements @ 17MPa and 35 o C Kaolinite Wettability

75 74
Advancing Advancing (T=20 C)
Advancing (T=35 C)
Receding
Advancing (T=65 C)
72 Receding (T=20 C)
Receding (T=35 C)
Receding (T=65 C)

Contact Angle (Degree)

Contact Angle (Degree)

70 70

68

66
65

64

62
60 0 5 10 15
0 5 10 15 20 25 30 35
Pressure (MPa)
Salinity (wt%)

Figure 6. Advancing and receding contact angles for CO2/water/kaolinite as a function of salinity (left) and pressure and
temperature (right).

smooth surface or report the surface roughness Carbon Dioxide/Water Interfacial Tension
conditions at each measurement. For the purpose of 90
Deionized Water (T=20 C)
this study, an average surface roughness of 45 nm Deionized Water (T=35 C)
was recorded by atomic force microscopy for the 80 Deionized Water (T=65 C)
Brine Water (T=20 C)
substrates used. Brine Water (T=35 C)
Interfacial Tension (mN/m)

70 Brine Water (T=65 C)

Interfacial Tension of CO2/Water 60

The presence of different monovalent (Na+ and

50
K ) or divalent (Mg2+, Ca2+) cations has impacts on
+

the interfacial tension (IFT) between CO2 and wa-

40
ter. For instance, IFT increases linearly with
increasing salt concentration with the IFT of a
solution containing divalent cations being at least 30

twice that of a solution with monovalent cations

(Baharuddin, 2013). The interfacial tension of CO2– 20
0 2 4 6 8 10 12 14 16
water system was measured at four different pres- Pressure (MPa)
sures (0.1, 5, 10 and 17 MPa) and at three temper-
Figure 7. CO2–water interfacial tensions as a function of
atures (20, 35 and 65 °C). The tests were carried out
pressure and temperature.
using deionized water and brine (NaCl 35 wt%) in
order to gain a better comparison of the salinity
effects. The results obtained indicated that the
interfacial tension initially decreases as the pressure di-Sia et al. (2007), Park et al. (2005), Georgiadis
increases, but it remains almost constant once the et al. (2010) and Espinoza and Santamarina (2010).
vapor–liquid boundary of CO2 is reached It was also found that the trend for deionized and
( 6.43 MPa at 24.85 °C) as shown in Figure 7. brine water is almost the same, but the interfacial
These findings were consistent with those of Sutjia- tensions recorded for the brine were generally
A Study on the Surface Wettability of Clastic Rocks

P = 17
T = 65
higher, a conclusion also reached by Espinoza and

42
36
23
20
74
72
Santamarina (2010).

P = 17
T = 35

33
22
20
17
71
68
Maximum Column Height of CO2

Knowing the type of rocks and their dominant

P = 17
T = 20

27
12
18
15
68
67
minerals, the following equation can be used to
determine the maximum column height of CO2
sustainable by any capillary seals before leakage

P = 10
T = 65

34
30
20
16
72
70
occurs.
2r  CosðhÞ
hmax ¼ ; ð2Þ

P = 10
T = 35
rgðqw  qCO2 Þ

26
19
17
13
69
67
Table 3. Advancing and receding contact angles of different CO2/brine/rock systems
where hmax is the maximum column height of CO2, r

P = 10
T = 20
is the interfacial tension, h is the contact angle, r is

24
10
13
11
67
65
the pore throat radius between the minerals, g is the
acceleration due to gravity, qw is the density of water

T = 65
and qCO2 is the density of CO2. In this study, the

P=5

27
25
17
14
70
68
differential density between water and CO2 was as-
sumed to be 350 kg/m3 (Iglauer et al. 2015), while

T = 35
the pore throat radii of the samples shown in Fig-

P=5

24
18
14
11
67
66
ure 1 were used. To determine the maximum col-
umn height, the contact angles and the interfacial
tension obtained at the temperature of 65 °C and the
T = 20
P=5

17

10

66
64
6

8
pressure of 17 MPa were considered. It is shown that
quartz- and feldspar-dominated sandstones can sus-
tain maximum column heights (CO2) of only 1 m
P = 0.1
T = 65

22
19
14
12
68
67
and 1.3 m, respectively. Kaolinite-dominated shale,
on the other hand, can sustain a 3900 m column
height (CO2) before leakage. These significant dif-
P = 0.1
T = 35

ferences in the column heights are mainly linked to

17
15
11

66
65
9

the pore throat sizes within the rocks and not their
surface wettability characteristics. In fact, quartz-
P = 0.1
T = 20

and feldspar-dominated sandstones are strongly

10

65
63
4
8
6

water wet rocks and provide a higher capillary

threshold pressure than shale. Thus, an accurate
Pressure (MPa)/Temperature (°C)

determination of the pore throat sizes present within

rocks surrounding a fault/seal is a much more
important parameter than the surface wettability
characteristics when considering seal integrity for
Advancing (Degree)

Advancing (Degree)

Advancing (Degree)

CO2.
Receding (Degree)

Receding (Degree)

Receding (Degree)

DISCUSSION

In this study, attempts were made to evaluate

the column height of CO2 sustained by capillary
seals. The measurements were made under different
Kaolinite
Feldspar
Quartz

pressure and temperature conditions with results

indicating that quartz- and feldspar-dominated
 B. A. Umar et al.

sandstones are strongly water wet under the differ- Petroleum Research and Development, Energy
ent pressure and temperature conditions, while Commission of Nigeria.
kaolinite-dominated shale becomes weakly water
wet when the pressure and temperature are ele-
vated. This indicates that residual trapping reduces
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