IPTC-21278-MS

A New Approach To Improve The Assessments of CO2 Geo-Sequestration

Capacity of Clay Minerals

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Emad A. Al-Khdheeawi, University of Technology-Petroleum Technology Department, Curtin University; Cut Aja
Fauziah, Curtin University; Doaa Saleh Mahdi, University of Technology-Petroleum Technology Department;
Ahmed Barifcani, Curtin University

Copyright 2021, International Petroleum Technology Conference

This paper was prepared for presentation at the International Petroleum Technology Conference held virtually on 23 March - 1 April 2021. The official proceedings
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Abstract
CO2 geological storage (CCS)isconsidered as the most promising technique to reduce atmospheric
CO2emissions. However, due to the density variation between the injected supercritical CO2 and the
formation water,CO2 tends to move vertically toward the air. This vertical CO2 leakage can be prevented
by four trapping mechanisms (i.e. structural trapping,capillary trapping, solubility trapping, and mineral
trapping). The capacities of structural and residual trapping are highly affected by rock wettability. Clay
wettability is one of the crucial parametersin evaluation of CO2 geo-sequestration. However, the literature
data show that there are many uncertainties associated with experimental measurements. One of these
uncertainties is the influenceof the effect of gas density on the clay mineral wettability. Thus, here, we
compared the wettability of a clay mineral (i.e. illite) of three different gas densities scenarios (i.e. low
(Helium), moderate (Nitrogen), and high (CO2) gas densities). To do so, we measured the advancing and
receding contact angle (i.e. wettability) of illite for CO2/water, nitrogen/water, and Helium/water systems
at a constant (333 K) and four different pressures (5, 10, 15, and 20 MPa). The brine composition used
was 4 wt% NaCl, 4 wt% CaCl2, 1 wt% MgCl2 and 1 wt% KCl, for all gas density scenarios. The results
indicate that gas density has a significant effect on the clay mineral wettability and that both advancing and
receding contact angles increase with an increase in gas density. The results show that a higher density gas
scenario has a higher contact angle of illite, measured at the same temperature and pressure. For instance,
the advancing contact angle of illite at 333 K and 20 MPa was 65° for the CO2/water system, 53° for the
nitrogen/water system, and 50° for Helium/water Helium/water system. Thus, we conclude that the gas
density affects the Clay wettability measurement and that the higher gas density leads to a higher contact
angle measurements (i.e. a more CO2-wet system) of the clay and thus reduces the estimated CO2 geo-
sequestration capacity and containment security.
2 IPTC-21278-MS

Introduction
Geological CO2 sequestration (GCS) is considered as a feasible technology for greatly mitigating global
climate change and reducing carbon dioxide emissions (Coninck et al., 2005; Lebedev et al., 2017; Yu et
al., 2017). There are three common options for CO2 geological storage, in terms of deep saline aquifers,
oil and gas reservoirs, and unmined-able coal beds (Al-Khdheeawi et al., 2018a-e; Al-Khdheeawi et al.,
2019). The fluid-fluid and fluid rock interfacial interactions mainly control successful subsurface storage
of carbon dioxide in deep saline aquifers and other types of hydrocarbon reservoirs. The Laplace equation
represents these interactions, where the main parameters to be considered are wettability and interfacial

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tension (Iglauer, 2011, Pentland et al., 2011, Morrow, 1990, Anderson, 1986, Arendt et al., 2004, Yang et
al., 2007, Chalbaud et al., 2009, Al-Khdheeawi et al., 2017a-e).
Some studies have been focused on wettability, especially clay wettability, through contact angle
measurements and researchers have found several discrepancies. Fauziah et al. (2018) have measured
contact angle between brine and CO2 on montmorillonite. According to the authors, there is an increase
in contact angle with increasing pressure; and montmorillonite is strongly oil-wet. Other researchers have
investigated the study on muscovite substrates (Chiquet et al., 2007, Farokhpooret al., 2013, Arif et al.,
2016) and organic shales (Barnet Shale) with mainly contained clay (Guiltinan et al., 2017, Pan et al., 2018,
Arif et al., 2017). The results show that the muscovite contact angles were increase while increasing pressure
and salinity, and decrease while increasing temperature. Meanwhile, organic shales contact angles changed
down with pressure, and change up with temperature. Pan et al. (2019a) have studied contact angles between
brine and methane on clay-coated quartz with the results show hydrophobicity increased with pressure
(elevated pressure) for clay-coated quartz. In addition, molecular dynamic simulations illustrate that Na-/
Ca-montmorillonite became more hydrophobic when exposed to CO2 at reservoir conditions (Myshakin et
al., 2013). To the best our knowledge, there is limited work on the correlation of gas density and pure clay
wettability found in the literature, even though this has been presented for quartz (Al-Yaseri et al., 2016,
Pan et al., 2019b).
In this paper, we analyse the correlation of gas densities and Illite wettability (pure clay) through contact
angle measurements. We measured carbon dioxide (CO2)/brine system for three different gas densities (i.e.
low (Helium), moderate (Nitrogen) and high (CO2) at various pressures (5 MPa, 10 MPa, 15 MPa and
20 MPa) and a constant temperature of 333 K. We then established new mathematical models to predict
advancing andreceding contact angles of Illite as a function of pressure and gas density. This model can be
utilised in reservoir simulation to develop GCS planning and to derisk the GCS projects.

Experimental methodology
The clay powder of Illite underwent mechanical compaction process to create solid sample. The material
used in this study was purely synthetic in nature. The clay powder was mixed with formation brine, which
consists of NaCl (20%wt), and KCl (1%wt) in deionised water. The mixture was then poured into cylinder
cell made of steel (in-house), with dimensions of 3.8 cm diameter by 10 cm length.
The mixture was cased inside a semi-permeable plate made of porous alumina, of 25% porosity, and an
average puresize of < 2 µm. Axial stressed 10 MPa was then applied on the mixture using a high precision
260D ISCO syringe pump with the excess brine was removedthrough a drainage tube. The sample was dried
at a temperature of 50°C for 48 hours.
The compacted sample was then used for contact angle measurement. The sample was kept in air plasma
for 5 minutes, to eliminate organic surface contamination. In using the tilted plate goniomteric technique
a HPHT (high temperature, high pressure) cell was designed. As described earlier, formation brine, which
consisted of NaCl (20%wt), and KCl (1%wt) in deionised water and mass fraction impurity of ≥ 0.99 was
used for the measurement. At a temperature of 333 K (60°C), the substrate was inserted into the cell. Three
different gas densities (i.e. low (Helium), moderate (Nitrogen) and high (CO2) were injected into the cell
IPTC-21278-MS 3

with a pressure accuracy of 0.1% FS, using a high precision pump (ISCO 500D), at preset pressures of
5 MPa, 10 MPa, 15 MPa, and 20 MPa. An equilibrated brine droplet of brine was then released onto the
substrate's surface through a needle. The detailed experimental setup has been described previously (Fauziah
et al., 2018; 2019; 2020). The process was recorded using a high-resolution video camera, with the images
from the film (movie files), reflecting both receding and advancing water contact angle. Standard deviation
from the contact angle measurements was ± 4º.

Results and discussion

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Effect of Gas Density on Illite Contact Angle
In this section we investigated the effect of gas density on the Iliite Contactangle (i.e. wettability). First we
measured the advancing and receding contact angle (i.e. wettability) of Illite for CO2/water, nitrogen/water,
and Helium/water systems at a constant (333 K) under four different pressures (5, 10, 15, and 20 MPa).
The brine composition used was 4 wt% NaCl, 4 wt% CaCl2,1 wt% MgCl2 and 1 wt% KCl, for all gas
density scenarios. Then, we compared the wettability of Illite with three different gas densities scenarios
(i.e. high (CO2), moderate (Nitrogen), and low (Helium) gas densities. The results indicate that gas density
has a significant effect on the Illite wettability and that both advancing and receding contact angles increase
with an increase in gas density (Figures 1 and 2 ). The results show that the higher gas density gas has
higher contact angle with Illite, measured at the same temperature and pressure. For example, the advancing
contact angle of Illite at 333 K and 5 MPa was 47º for the CO2/water system while it was 26º for the Helium/
water system (Figure 1). Thus, we conclude that the gas density affects the Illite wettability and that higher
gas density leads to increase the CO2-wettability of the clay.

Figure 1—Illite advancing contact angle as a function of gas density measured at temperature of 333 K.
4 IPTC-21278-MS

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Figure 2—Illite receding contact angleas a function of gas density measured at temperature of 333 K.

Predicting of Illite Contact Anglefrom Gas Density

In this section, we used our measured contact angle to developed new correlations for predicting advancing
and receding contact angles for the Illite as a function of gas density. Our results show that the Illite
advancing and receding contact angles can be predicted from gas density using the following second degree
polynomial equations:
(1)
(2)
Where:
θ:Contact Angle ∘ ρ: Gas density kg/m 3
These new equations (Eq. 1 and2) predict the advancing and receding contact angles of Illite as a function
of gas density with very good accuracy (i.e. correlation coefficient (R) was 0.87 and 0.86 for equations 1
and 2, respectively (Figures 3 and 4).
IPTC-21278-MS 5

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Figure 3—Cross-plot of the experimental and calculated advancing contact angle (using equation 1) for Illite.

Figure 4—Cross-plot of the experimental and calculated receding contact angle (using equation 2) for Illite.

Conclusion
CO2 geological storage capacity is highly affected by rock wettability. Clay wettability is one of the crucial
parameters in evaluation of CO2 geo-sequestration. Literature data show that there are many uncertainties
associated with clay experimental measurements. One of these uncertainties is the effect of gas density on
the Illite wettability. Thus, here, we investigated the effect of gas density on Illite contact angle. Our results
6 IPTC-21278-MS

indicate the gas density has a clear effect on the Illite contact angle and that increasing gas density leads
to increase the contact angle of Illite. In addition, we have proposed new equations to predict advancing
and receding contact angles for Illite as density at a constant temperature a function of gas density. This
implication can be utilised to improve the wettability predictions, and thus, the assessments of CO2 geo-
sequestration capacity.

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