Journal of CO2 Utilization 72 (2023) 102507

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Journal of CO2 Utilization

journal homepage: www.elsevier.com/locate/jcou

Experimental evaluation of foams stabilized by ionic liquids for enhanced

oil recovery
Alba Somoza a, Ana Soto a, Jieqiong Pang b, Kishore K. Mohanty b, *
a
CRETUS. Department of Chemical Engineering, Universidade de Santiago de Compostela, E-15782 Santiago de Compostela, Spain
b
Hildebrand Department of Petroleum and Geosystems Engineering, The University of Texas at Austin, 200 E. Dean Keeton Dr., Austin, TX 78712, USA

A R T I C L E I N F O A B S T R A C T

Keywords: Foam injection has the potential to improve CO2 enhanced oil recovery (EOR) and simultaneous CO2 seques­
Ionic Liquids tration processes by increasing sweep efficiency. However, the stability of the foam remains a challenge specially
CO2 enhanced oil recovery at harsh conditions of temperature, pressure, and salinity. Surface-active ionic liquids (SAILs) are promising
Foam stability
chemicals that usually exhibit high surface activity, salinity tolerance, and thermal stability. This study in­
Apparent viscosity
CO2 sequestration
vestigates the performance of SAILs to produce foam for CO2 EOR in two high salinity reservoirs (A and B). Both
reservoirs are at high salinity conditions with salinities of 125,356 mg/L and 255,470 mg/L. Half-life time and
initial foam height were considered to represent foam stability and foaming ability, respectively. An optimal
formulation of 0.5 wt% [C16mim]Cl was selected for reservoir A conditions, whereas 0.5 wt% [C16Py]Cl and 0.5
wt% [C16mim]Cl formulations were studied for reservoir B conditions. Foam mobility was measured at a quality
of 80% to test the validity of the proposed formulations. A promising half-life of 7.8 days was obtained for
[C16mim]Cl at Reservoir A conditions in high-pressure stability tests, several times higher than those reported in
literature for traditional surfactants. Mobility reduction factors higher than 300 were reported for all the cases,
with the most promising result (1229) achieved for [C16mim]Cl at Reservoir A conditions. These results indicate
that strong foams can be generated at high salinity conditions using SAILs. This work shows the promising
possibilities of SAILs to improve the sweep efficiency in CO2-EOR methods and enhance the gas trapping in
sequestration processes.

1. Introduction sequester CO2 in underground formations previously occupied by oil

[4]. However, the large viscosity contrast between gas and both oil and
Primary and secondary stages of oil production from conventional water during CO2 injection usually results in early gas breakthrough and
reservoirs produce an average of 30% of original oil in place, leaving a poor sweep efficiency. Even in CO2 sequestration in aquifers, viscous
high percentage of oil behind [1]. With the decline in oil production fingering phenomenon is also a significant challenge, as it can impact
from mature reservoirs and the global oil demand set to increase, the long-term storage capacity in underground formations. Injection of
improving oil recovery is still a major issue. In this context, tertiary or gas in the form of foam can help to overcome these issues [5].
enhanced oil recovery (EOR) methods are developed to improve oil Foam is a dispersion of gas bubbles in a water phase produced in the
production. EOR techniques usually involve injection of chemical solu­ presence of a foaming agent (surfactant). Each bubble is separated by
tions (surfactant or polymer EOR), gases (miscible or immiscible EOR), thin liquid films called lamellae [6]. Foam reduces the mobility of gas by
or high-temperature fluids such as steam or hot water (thermal EOR) increasing the apparent gas viscosity and reducing gas relative perme­
[2]. Gas flooding is a widely used EOR method; oil can be displaced by ability [7]. Several surfactants have been proposed to stabilize foams in
different gases, such as, carbon dioxide, hydrocarbon gas, nitrogen, or field applications [8]. However, stability of the foam at harsh conditions
flue gas [3]. In this context, CO2 injection is attracting new market in­ of temperature, pressure and salinity is still a challenge. At these con­
terests since it is considered a promising way to ensure cost-efficient ditions, the rapidly thinning out of the lamellae by film drainage and
avoidance of CO2 emissions to atmosphere. This technology can pressure difference between bubbles cause inter-bubble gas diffusion
generate a product with a strong economic value while it can also and subsequent bubble rupture (coalescence), thus de-stabilizing the

* Corresponding author.
E-mail address: kishore.mohanty@engr.utexas.edu (K.K. Mohanty).

https://doi.org/10.1016/j.jcou.2023.102507
Received 7 March 2023; Received in revised form 21 May 2023; Accepted 22 May 2023
Available online 25 May 2023
2212-9820/© 2023 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-
nc-nd/4.0/).
A. Somoza et al. Journal of CO2 Utilization 72 (2023) 102507

foam. A limited number of studies have been conducted on CO2 foam 255,470 mg/L salinity, and 1000 psi). Aqueous stability and bulk foam
performance under harsh reservoir conditions. Some authors [9–13] stability experiments at ambient pressure are carried out, aiming to test
studied the influence of temperature and pressure on CO2 foams stabi­ the performance of the different foams and select the most promising
lized by surfactants through foam stability and foam mobility tests. As a SAILs. Finally, the effectiveness of the proposed SAIL formulations is
general conclusion, all the studies agreed that foam lifetime decreases evaluated via high-pressure stability studies and foam mobility tests. Air
with temperature, but the effect of pressure was complex to evaluate. but also, for the first time, CO2 is selected as foaming gas in combination
Wang et al. [9] found out that the influence of this variable greatly with SAILs. Foam apparent viscosity and mobility reduction factor are
depends on the type of surfactant used. In addition, Zhang et al. [10] and determined. This work offers a significant advance in the application of
Wang et al. [11] claimed that, at the same conditions, foam stability SAILs in CO2 EOR processes.
achieved with higher alkyl chain length was better than with shorter
alkyl chain length surfactants. The effect of salinity has also been 2. Materials and methods
assessed by several authors [8,14,15]. Studies agreed that foam stability
is higher at higher salt concentrations due to the reduction of the elec­ Six different cationic SAILs with the most common functional groups
trostatic repulsion between surfactant molecules making the lamellae (ammonium, imidazolium and pyridinium) were selected for this study.
rigid. Nevertheless, in all these studies, half-life time of CO2 foams sta­ Cocosalkylpentaethoximethylammonium methylsulfate (C1EG) and N,
bilized with surfactants did not exceed 300 min. Therefore, it is desirable N-diethoxylated-N-tallow-N-ethylammonium ethylsulfate (T2EG) were
to develop CO2 aqueous foams with improved stability at high temper­ supplied by Iolitec with a purity > 95 wt%. T2EG has a higher alkyl
ature, salinity, and pressure conditions. chain length and ethoxylation degree than C1EG which results in higher
Recently, some researchers have investigated the use of ionic liquids hydrophilicity compared to C1EG. Two different alkyl chain lengths (C12
(ILs) as alternative chemicals in enhanced oil recovery processes and C16) were studied for pyridinium and imidazolium SAILs. N-Dode­
[16–18]. Surface active ionic liquids can reduce the surface tension of cylpyridinium chloride (purity ≥ 93 wt%) and hexadecylpyridinium
water to about 30–40 mN/m [19]. The water-crude oil interfacial ten­ chloride monohydrate (purity ≥ 99 wt%) were purchased from Sigma
sion can be reduced to about 1 mN/m from about 40 mN/m by the Aldrich. 1-Hexadecyl-3-methylImidazolium chloride and 1-Dodecyl-3-
addition of ionic liquids [20]. These compounds are salts with melting or methylimidazolium bromide both with a purity > 98 wt% were sup­
glass transition temperatures below 100 ◦ C. Their negligible vapor plied by Iolitec. Their most important characteristics are listed in
pressure, high thermal stability and high solvating capacity makes them Table 1. Density and viscosity at 25 ◦ C and atmospheric pressure were
ideal compounds for the application. In addition, cations and anions of determined for liquid compounds using an Anton Paar DMA 5000 M
these salts can be selected to design task-specific compounds that meet density meter and an Anton Paar LOVIS 2000 ME microviscometer,
the requirements of each specific reservoir. In comparison to traditional respectively. Before measuring physical properties, water content of the
surfactants, it has been proven that ILs show advantages regarding sta­ corresponding SAILs was measured using Karl-Fischer titration in a
bility at high salinity and temperature conditions [20,21]. In this Metrohm 899 coulometer. Water content values of 896.1 ppm and
context, ILs seem promising candidates to overcome stability problems 723.3 ppm were obtained for C1EG and T2EG, respectively.
of CO2 foams. The application of these chemicals in the conditions of two different
Only a few researchers have investigated the use of ILs in EOR foam reservoirs was studied in this paper. Reservoir A is in Canada and its
applications. Hu et al. [22] and Ouyang et al. [23] studied the effect of conditions are 63 ◦ C and 1910 psi. Reservoir B is located in Michigan
imidazolium ILs structure on foam features using Density functional (United States) and it is characterized by a temperature of 40 ◦ C and a
theory (DFT) simulations and foam stability experiments. They pressure of 1000 psi. Formation brines of each reservoir were prepared
concluded that the introduction of hydroxyl groups and longer alkyl by dissolving different amounts of salts in distilled water with the
chain lengths in the imidazolium cation was favorable for foam features. compositions shown in Table 2. They are both high salinity reservoirs.
More applied approaches can also be found in the Literature. Sakthivel Sodium chloride, potassium chloride, calcium chloride dihydrate,
and Salin [5] studied the use of imidazolium ILs, with varying alkyl magnesium chloride hexahydrate, sodium carbonate and sodium bi­
chain length, as additives to a non-ionic surfactant to improve foam carbonate were ACS certified and purchased from Fisher Chemicals.
stability. They performed bulk and porous-scale dynamic foaming ex­ CO2 with a purity of 99.9 wt% was purchased from Linde Gas &
periments at high-pressure (2200 psi) and high-temperature (80 ◦ C). Equipment. Ottawa sand F95 was used in sand-packs; it was obtained
Stability of the foam in the presence of IL increased by more than 50% from US Silica.
compared to their neat surfactant solution. They also concluded that, as
in the case of traditional surfactants, longer alkyl-chain exhibited higher 2.1. Compatibility tests
stability and higher foamability than shorter alkyl-chain ILs. However,
even though they tested different gases in bulk foam experiments, they The compatibility of SAILs with Canada and Michigan brines, at both
only worked with N2 in porous media tests. Deep eutectic solvents ambient and reservoir temperatures, was evaluated. To that aim, 10 mL
(DESs), constituted by choline chloride and two short-alkyl chain imi­ of 0.5 wt% SAIL in the corresponding formation brine were prepared in
dazolium ILs, were employed by Hanamertani et al. [24] as additives to glass vials and visually monitored for 1 week. To check the stability at
a mixture of anionic and amphoteric surfactants. Bulk foam experiments reservoir conditions, the vials were placed in an oven operating at 40 ◦ C
at ambient and high temperature (80 ◦ C) were performed to study foam (B) or 63 ◦ C (A). Optically clear samples were considered stable, while
stability. Results showed that ILs and DESs were able to improve sur­ cloudy or precipitated samples were considered unstable.
factant foam stability. In their subsequent work [25], the most prom­
ising ILs and DESs were tested on dynamic foam mobility test using N2 as 2.2. Static foam experiments
the foaming gas. Unfortunately, permeability of the core, flow rate and
temperature and pressure conditions were not reported. All these results Static foam experiments were performed to compare the foaming
provide an indication of the capability of ILs to reduce gas mobility and ability of the proposed SAILs. These tests are a fast-screening method to
increase mobility reduction factor during injection processes. evaluate the suitability of the different surfactants for the application. In
In this paper, six surface-active ILs (SAILs) with the most common this study, initial foam height and foam stability were assessed over
functional groups are tested for CO2 foam EOR. The influence of the time. Two foaming gases were screened: air and CO2. Experiments were
alkyl chain length and ethoxylation degree on the SAILs performance is performed at 40 ◦ C (B) and 63 ◦ C (A) according to each reservoir
analyzed. Two different reservoir conditions are evaluated: Reservoir A temperature.
(63 ◦ C, 125,356 mg/L salinity, and 1910 psi) and Reservoir B (40 ◦ C, Foam was prepared according to the methodology developed in

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A. Somoza et al. Journal of CO2 Utilization 72 (2023) 102507

Table 1
SAILs used in this study.
Abbreviature Compound Chemical structure Appearance Molecular CMC Density at Viscosity
Weight (g/ 25 ◦ C (g/ at 25 ◦ C
mol) cm3) (mPa⋅s)

C1EG Cocosalkylpentaethoximethylammonium Liquid Not 88.1 mg/L 1.085466 2477.6

methylsulfate available [26]

T2EG N,N-Diethoxylated-N-tallow-N- Liquid Not 36.32 mg/L 1.077613 609.25

ethylammonium ethylsulfate available [27]

[C12Py]Cl N-Dodecylpyridinium chloride Solid 283.88 15.27 mmol/ - -

L[28]

[C16Py] Hexadecylpyridinium chloride Solid 358.00 1.22 mmol/L - -

Cl⋅H2O monohydrate [29]

[C12mim]Br 1-Dodecyl-3-methylimidazolium bromide Solid 331.34 10.6 mmol/ - -

kg[30]

[C16mim]Cl 1-Hexadecyl-3-methylimidazolium Solid 343.00 0.99 mmol/L - -

chloride [29]

2.3.1. High pressure stability study

Table 2
Promising SAILs according to static foam experiments were tested by
Formation brines composition.
means of high-pressure stability tests. Bulk foam experiments were
Ion Reservoir A (Canada) Reservoir B (Michigan) carried out in a high-pressure view cell to check foam stability at
Na+ 29,900 mg/L 51,802.3 mg/L reservoir conditions of pressure and temperature. For these experiments,
K+ 4210 mg/L 5286.32 mg/L the system was initially vacuumed for 2 h and then pre-flooded with
Ca2+ 12,000 mg/L 32,697.7 mg/L
surfactant solution at a constant injection rate of 5 mL/min. Subse­
Mg2+ 2020 mg/L 5898.2 mg/L
Cl- 79,000 mg/L 152,318 mg/L
quently, pressure of the system was increased to the target pressure.
HCO-3 896.7 mg/L 152.5 mg/L Surfactant formulation and CO2 gas were co-injected through a foam
SO2-4 690 mg/L 4763.505 mg/L generator into the high-pressure view cell. A 7 µm filter was used as
Total salinity 125,356 mg/L 255,470 mg/L foam generator. Flow rates of 0.4 mL/min of surfactant solution and
1.6 mL/min of CO2 were stablished for a nominal foam quality of 80%.
previous studies [31,32]. 2 mL of 0.5 wt% SAIL solution in the corre­ Surfactant concentration was set to 0.5 wt% in the corresponding brine.
sponding brine were placed in sealed tubes of 15 mL. The tubes were Pictures of the high-pressure cell were taken inside the oven at different
heated in an oven for several hours until reaching the target tempera­ times. The foam height above the liquid was determined using image
ture. Foam was produced by hand shaking the solution for 2 min until analysis software. Half-life time was calculated as the time for which the
foam height was constant. The decay of foam volume was monitored as a foam is reduced to half of its original volume.
function of time until the foam disappeared. The time for which the
volume of foam is reduced to half of its original volume is known as the 2.3.2. Foam mobility test
half-life time. Experiments were repeated twice to ensure repeatability Foam-flow experiments were performed in a sand-pack to investigate
and average half-life time and initial foam height were reported. the ability of the foam created by the most promising SAILs to reduce
mobility at reservoir conditions. The primary objective was determining
2.3. Gas-surfactant co-injection experiments the steady state pressure drop across the sand-pack, to estimate the
mobility reduction factor (MRF) and apparent foam viscosities (µaf). To
The experimental set-up used for high pressure stability and foam that aim, a vertically oriented stainless-steel column, 30.48 cm length
mobility tests is shown in Fig. 1. The equipment contained two ISCO and 2.225 cm internal diameter, was uniformly packed with dry sand.
pumps and two accumulators for SAIL solution and CO2 injection. A After packing the sand column tightly, pore volume (PV) and
sand-pack and a high-pressure view cell were connected in two parallel permeability of the sand-pack were determined. To this effect, the col­
circuits to work with one of them while keeping the other circuit closed. umn was vacuumed for 24 h and flooded with distilled water at constant
A back pressure regulator (BPR) was used to maintain the system pres­ pressure. PV was calculated by measuring the volume of water required
sure at either 1000 or 1910 psi. All the equipment was kept inside an to saturate the column. The saturated sand-pack was then flooded with
oven to perform experiments at the reservoir temperature (40 ◦ C or distilled water, at different flow rates, to record the corresponding
63 ◦ C). A pressure transducer was used to monitor pressure drop. pressure drops and determine the absolute permeability using Darcy’s
law. Water was removed by heating and vacuuming the sand-pack.
The sand-pack was then introduced in the equipment, vacuumed for
2 h, and pre-flooded with 2 PV of surfactant solution at a constant

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A. Somoza et al. Journal of CO2 Utilization 72 (2023) 102507

Fig. 1. Experimental set-up for high pressure stability and foam mobility tests.

injection rate of 5 mL/min (to avoid the influence of surfactant The effective viscosity of the foam, µaf was calculated using (based on
adsorption in the subsequent experiments). Surfactant concentration in Darcy’s law):
formation water was 0.5 wt%. Pressure of the system was increased to
ΔPsurf +gas ⋅k⋅A
the target pressure. Subsequently, CO2 and surfactant formulation were µaf = , (2)
q⋅L
co-injected at 80% foam quality from the top of the sand-pack. Total
flow rates of 0.122 mL/min (4 ft/day) and 0.304 mL/min (10 ft/day) where k is the absolute permeability of the porous medium, A and L are
were studied. Pressure drop (ΔP) was recorded using a pressure trans­ the area and length of the sand-pack and q is the total flow rate of sur­
ducer until it remained constant. Distilled water was injected through factant and gas.
the sand-pack at a constant pressure after each test to clean it. Perme­
ability was checked to ensure its consistency through the different 3. Results and discussion
experiments.
MRF is defined as the ratio of the pressure drop in the presence of 3.1. Compatibility tests
foam to the pressure drop during surfactant solution injection [33], i.e.,
ΔPsurf +gas The compatibility of six different SAILs in the formation brines
MRF = . (1) shown in Table 2 was tested at various conditions. As it can be seen in
ΔPsurf
Fig. 2, no precipitation or cloudiness was observed for any SAIL at the

Fig. 2. Stability tests. Pictures taken after 1 week.

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A. Somoza et al. Journal of CO2 Utilization 72 (2023) 102507

reservoir temperature after one week. However, [C16mim]Cl and (0.34 min) and H0 (4.35 cm) of T2EG were lower than for C1EG
[C16Py]Cl precipitated after one week at the ambient temperature in (0.47 min and 11.15 cm). Although T2EG has longer alkyl chain length
both brines. The aqueous solubility of ILs generally increases with than C1EG, the higher ethoxylation degree results in higher hydrophi­
temperature [34] and decreases with the alkyl chain length size [35]. licity. This increase in hydrophilicity, is believed to cause the weakening
Since all the SAILs were stable at reservoir temperature, they were of the arrangement of surfactant molecules at the interface, due to the
considered for further tests. strong interactions with water, and thereby weaken the liquid film of the
foam [8].
Ideally, a surfactant for EOR should have both, good foamability and
3.2. Static foam experiments
foam stability. However, in some cases, it may be necessary to prioritize
one property over the other [38]. In general, when dealing with high
Static foam experiments were performed to compare foam ability
temperature, pressure or salinity conditions, foam stability may become
and bulk foam stability of SAIL formulations. Foams are thermody­
a more critical factor to consider, as the high temperature and salinity
namically unstable, and eventually collapse due to gravity drainage of
can cause surfactant degradation and lead to foam collapse over time
the liquid film and diffusion through gas bubbles, also known as Ostwald
[9]. As a result, selecting a surfactant with good stability properties, can
ripening. When ionic surfactants like the SAILs tested in this paper are
help to improve the longevity and effectiveness of the foam in the
used as surface active agents, the liquid film is charged. Therefore, the
reservoir. For this reason, [C16mim]Cl was selected as the most prom­
overlapping of similarly charged electric double layers opposes film
ising SAIL for reservoir A conditions since it showed the highest half-life
thinning, thus strengthening the stability of foam [36]. Foaming ability
time and acceptable initial foam height.
was measured by means of the initial foam height (H0), and half-life time
In Table 4 results of H0 and half-life time for the different SAILs at
was used to determine foam stability. The study was performed for the
reservoir B conditions are shown. Reservoir B temperature is lower
two reservoir (A and B) conditions of salinity and temperature. SAIL
(40 ◦ C) and salinity higher (255,470 mg/L TDS) than reservoir A (63 ◦ C
concentration was fixed at 0.5 wt%, as it is a typical surfactant con­
and 125,356 mg/L TDS). As a general remark, the results from these
centration used in field applications [31]. Two different foaming gases
tests indicate that foaming ability decreases and foam stability increases
(air and CO2) were studied. Measurements were repeated twice, and
when switching from reservoir conditions A to B. It is known that tem­
mean deviation was less than 10% for half-life time results and less than
perature has little impact on foaming ability, whereas it significantly
5% for H0 values.
affects foam stability. Nonetheless, as general rule, the higher the tem­
Table 3 shows H0 values and half-life times for the different SAILs at
perature, the less stable is the foam [39]. On the other hand, salinity is a
reservoir A conditions. Air based foams were found more stable than
major factor affecting foam ability and stability due to the interaction
CO2 foams, as it was expected due to the higher solubility of CO2 in the
between electrolytes and surfactant molecules at the interface [8].
foaming solution [5]. Solubility of gases in water has a negative effect on
Several authors have studied the effect of salinity on foam performance.
foam stability because it can accelerate the foam coalescence [9]. The
Kumar and Ghosh [40] have tested several surfactants and reported the
effect of the different SAILs on the analyzed parameters was the same
existence of an optimum salinity for each compound. They showed that
regardless of the foaming gas. Focusing on CO2 EOR, due to the envi­
a minimum surface tension of the aqueous solution is the key parameter
ronmental benefits of the method, the discussion in this section refers to
for good foaming. A little increase in foam height at very low concen­
the numerical values of CO2 foam. A H0= 5.75 cm and half-life time of
trations of NaCl was observed. However, NaCl decreased the foam
5.27 min were achieved with the SAIL [C16mim]Cl. Half-life time was
height at moderate and higher concentrations. Varade and Ghosh [15]
significantly lower (0.69 min) in the case of [C12mim]Br, but H0 was
and Behera et al. [41] found out that H0 decreases with the increase of
remarkably higher (9.95 cm). A similar result was obtained with the
salt concentration. The reason for this reduction in foam volume is
SAILs [C16Py]Cl and [C12Py]Cl. Therefore, longer alkyl chain length
proposed to be the fast coalescence rate of bubbles due to the reduction
compounds resulted in a lower foaming ability, but a higher stability.
in the electrostatic double layer repulsion. Xu et al. [14] found that
These results are in agreement with other studies previously carried out
stability increases with salt concentration due to the formation of
with different ILs. Hu et al. [22] studied the foaming performances of
smaller and more stable bubbles. They claimed that high salt concen­
different alkyl chain length imidazolium ILs. They found that the H0 was
trations reduce the electrostatic repulsion between surfactant molecules,
lower for C8 than for C6 ILs. They claimed that this reduction is probably
which facilitates its adsorption on the film, making the lamellae rigid. As
caused by the increase of hydrophobic groups, that leads to the decrease
a result, the film thinning rate is reduced and stability increased. These
of solubility in water, resulting in an inferior foaming performance. They
findings are in accordance with our results. Foaming ability was found
also concluded that the longer the alkyl chain length, the higher the
lower and foam stability higher at the lower temperature and higher
foam stability. Zhang et al. [37] found that the longer the alkyl chain
salinity conditions.
length, the stronger is the interaction between molecules, resulting in
[C16mim]Cl and [C16Py]Cl gave the higher foam stability at reservoir
greater external forces required for the bursting of foam, and therefore a
B conditions. However, [C16mim]Cl initial foam height was considered
more stable foam. Comparing SAILs functional groups, pyridinium SAILs
too low. Considering that salinity is the major factor affecting foam
showed better foaming ability, but lower stability than imidazolium
ability, a new attempt using half the concentration of the formation
compounds.
brine at the same temperature was made. Table 5 shows the results of
C1EG and T2EG are two quaternary ammonium SAILs. Half-life time

Table 3 Table 4
Static foam test results for reservoir A. Static foam test results for reservoir B.
[C16mim] [C16Py] [C12mim] [C12Py] C1EG T2EG [C16mim] [C16Py] [C12mim] [C12Py] C1EG T2EG
Cl Cl Br Cl Cl Cl Br Cl

Air Air
H0 (cm) 6.5 7.25 9.3 10.5 11 4.15 H0 (cm) 2.35 4.95 10 10.45 8.35 2.85
Half-life 21.80 17.20 2.53 1.24 1.99 0.72 Half-life 81.25 54.74 7.81 4.72 6.13 16.64
(min) (min)
CO2 CO2
H0 (cm) 5.75 5.9 9.95 12.05 11.15 4.35 H0 (cm) 2.95 4.6 10.15 11.85 8.65 5.35
Half-life 5.27 3.58 0.69 0.53 0.47 0.34 Half-life 8.60 3.37 1.94 1.58 0.87 0.67
(min) (min)

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A. Somoza et al. Journal of CO2 Utilization 72 (2023) 102507

Table 5
Static foam test results for reservoir B using half concentration of formation
brine.
[C16mim]Cl

Air CO2
Height (cm) 3.8 3.95
Half-life (min) 19.47 4.36

static foam tests for [C16mim]Cl at these new conditions. The salinity
decrease caused a reduction in half-life time from 8.60 min to 4.36 min.
However, initial foam height was increased from 2.95 cm to 3.95 cm.
For reservoir B, further tests were performed using [C16Py]Cl and
[C16mim]Cl with half formation brine salinity.
Although stability tests were not performed in the presence of crude
oil, it should be mentioned that crude oil can negatively impact foam
stability by reducing surface tension, destabilizing foam lamellae, and
coalescing foam bubbles. This can result in a decrease of foam height, Fig. 4. High pressure stability study of [C16Py]Cl for reservoir B project.
shorter foam lifetime, and therefore lower foam stability [42]. Further
studies, out of the scope of this paper, are required to determine the of [C16mim]Cl, foam stability was 4 times higher than for the pyridinium
compatibility of the foam with crude oil. Regarding adsorption in porous IL. Foams produced with the imidazolium SAIL showed smaller bubbles
media, Nandwani et al. [43] studied the adsorption mechanism of and a more uniform bubble size distribution than in the case of the
several SAILs (imidazolium, pyridinium and pyrrolidinium) on different pyridinium SAIL. Generally, more uniform and smaller bubble sizes lead
rock types under high salinity conditions. Lower adsorption of SAILs was to high stability of the foam due to reduced Ostwald ripening and coa­
observed for crushed carbonate than for sandstone samples, reporting lescence [44].
lower values than those found for the conventional cationic surfactant Foam stability of [C16mim]Cl at reservoir A conditions is consider­
CTAB. The imidazolium-based SAIL showed the minimum adsorption ably higher than for reservoir B conditions. It should be noted that in
among the SAILs studied. They concluded that the increase of temper­ both cases salinity is ~125,000 ppm of TDS since half concentration of
ature and salinity, leads to a decrease of the amount of SAIL adsorbed on reservoir B formation brine was applied. Reservoir A conditions of
both types of rocks. Electrostatic repulsion is the basic mechanism for pressure and temperature (63 ◦ C and 1910 psi), unlike reservoir B
low adsorption of SAILs in carbonate rocks. conditions (40 ◦ C and 1000 psi), are above the CO2 critical point
(31.1 ◦ C and 1068.93 psi). When temperature and pressure conditions
exceed this critical point, gaseous CO2 transformed into a liquid-like
3.3. High pressure stability study
fluid with a density significantly higher than that of gaseous CO2, thus
reducing the water drainage from lamellae [45].
In order to use foams in tertiary oil production, the dispersion of CO2
It is known that as pressure increases, the solubility of CO2 in brine
bubbles in surfactant solution must be stable at the harsh conditions of
increases according to Henry’s Law, with a negative effect on foam
the studied reservoirs, including not only high salinity and temperature
stability. However, at high pressures, the density of CO2 increases due to
but also high pressure. For this reason, bulk foam experiments at pres­
the compression of gas [9]. The density increase lowers the liquid
sure conditions of each reservoir (1910 psi for A and 1000 psi for B)
drainage and stabilizes foam. We observed that the half-life increases
were performed in a high-pressure cell to determine foam stability.
with pressure implying that the density effect was more important than
Fig. 3 shows the stability study for [C16mim]Cl at reservoir A conditions.
the solubility effect for SAIL foams. However, there is no agreement in
Rate of foam decay was low and half-life time was estimated as 7.8 days,
the literature about how pressure affects CO2 foams stability. Some
several times higher than those reported in literature for regular sur­
authors concluded that stability increases with pressure [10,46],
factants at similar conditions [11]. Figs. 4 and 5 present the high pres­
whereas other authors claimed that it decreases [47,48]. Furthermore,
sure stability study at reservoir B conditions for [C16Py]Cl and [C16mim]
Szabries et al. [44] studied foam stability of Triton X-100, a non-ionic
Cl (half formation brine salinity), respectively. Half-life time for [C16Py]
surfactant, at 45 ◦ C and for a pressure range of 0–1233 psi. The au­
Cl was estimated as 0.98 h and for [C16mim]Cl, 4.5 h. Salinity has a
thors found that, between 0 and 1087 psi, stability decreased with
positive effect in foam stability. Although salinity was lower in the case

Fig. 3. High pressure stability study of [C16mim]Cl for reservoir A project.

6
A. Somoza et al. Journal of CO2 Utilization 72 (2023) 102507

Fig. 5. High pressure stability study of [C16mim]Cl for reservoir B project using half concentration of formation brine.

increasing pressure. However, the contrary behavior was found between foam. Injection rate should be greater than the critical injection velocity
1087 and 1233 psi, and foam stability improved with increasing pres­ to obtain a stable foam. The minimum pressure gradient for mobilization
sure. In accordance with our results, Zhang et al. [10] found out that of liquid lamellae and foam generation depends on different factors such
foams of tertiary amines were more stable with rising CO2 density. as permeability of the medium, surfactant type and concentration, gas
The behavior of CO2 foam stability with pressure is complex, with type and foam quality [3]. The velocity of 4 ft/day is likely below the
different classes of surfactants behaving differently with pressure. Wang critical velocity of the system, and therefore results were discarded.
et al. [9] and Zhang et al. [10] concluded that the effect of pressure on For tests performed at a total injection rate of 0.304 mL/min, values
foam stability depends on the hydrophilic-lipophilic balance (HLB) of of differential pressure as a function of pore volume (PV) injected are
the surfactant used. The solvation of hydrocarbon tails increases with presented in Fig. 6. A steady-state pressure drop was observed after
the density of CO2, as it becomes more hydrophobic. As a result, strong 1–1.4 PV, indicating the absence of plugging. The average final value
surfactant hydrophilic heads are needed to balance this interaction. was used to calculate MRF and µaf according to Eqs. 1 and 2. Values of
However, if the surfactant is too hydrophilic it can be embedded into the average steady-state pressure drop, MRF and µaf for each case studied are
water phase and weaken the liquid film. On the contrary, surfactants reported in Table 7.
with low HLB values can disorder the arrangement of surfactant mole­ The highest pressure drop recorded was 115.97 psi corresponding to
cules leading to unstable foams. In conclusion, for surfactants with [C16mim]Cl at reservoir A conditions. Regarding reservoir B conditions,
relatively high HLB values, high pressures can increase the interaction a differential pressure of 52.86 and 25.60 were obtained for [C16mim]Cl
between surfactant molecules and CO2, making the foam to be at the (using half salinity of formation brine) and [C16Py]Cl, respectively.
most stable state. In this state, the arrangement of the molecules at the Mobility reduction factor varied from 300 to 1230. In accordance with
interface is tightened and foam stability is improved by reducing water results from high pressure stability studies, the higher the half-life time
drainage and gas diffusion [9]. In this study, [C16mim]Cl and [C16Py]Cl the higher the mobility reduction factor in porous media. Foam apparent
are two hydrophilic surfactants with long carbon chains, therefore the viscosity was also calculated to characterize foam flow. It should be
hydrophilicity is not as high as for other surfactants with shorter alkyl noted that apparent viscosity of foam depends on foam velocity. The
chains. For the three cases studied, stability was improved with apparent viscosity decreases as the foam velocity increases [53]. This is
increasing pressure comparing half-life time at atmospheric (Section probably due to the shear-thinning behavior commonly observed in
3.2) and reservoir pressure. In addition, the highest stability was re­
ported for the highest reservoir pressure (reservoir A).

3.4. Foam mobility test

Foam-flow experiments in the absence of oil were conducted in a

vertically oriented sand-pack column. Pore volume, porosity and
permeability of the sand-pack are presented in Table 6. SAIL concen­
tration was kept at 0.5 wt%. Experiments were performed at 80% foam
quality for each reservoir conditions of pressure and temperature. Total
flow rates of 0.122 mL/min (4 ft/d) and 0.304 mL/min (10 ft/d) were
studied, however unstable values of pressure difference were observed
for 0.122 mL/min. Several researchers [49–52] have investigated the
importance of a critical injection velocity (related to a minimum pres­
sure gradient) in porous media for transition from “coarse” to “strong”

Table 6
Sand-pack properties.
Property Value

Pore volume (mL) 43.84 Fig. 6. Foam mobility tests for [C16mim]Cl reservoir A (▫), [C16Py]Cl reservoir
Porosity (%) 36.99
B (•) and [C16mim]Cl reservoir B using half concentration of formation
Permeability (mD) 6828.04
brine (▴).

7
A. Somoza et al. Journal of CO2 Utilization 72 (2023) 102507

Table 7 Co-directed research and edited manuscript. Jieqiong Pang: Conducted

Results of sand-pack experiments. experiments, helped with manuscript. Kishore Mohanty: Directed
ΔP (psi) MRF µaf (cp) research, edited manuscript.
[C16mim]Cl reservoir A 115.97 1229.01 1356.61
[C16mim]Cl reservoir B (1/2 FB) 52.86 560.19 618.35 Declaration of Competing Interest
[C16Py]Cl reservoir B 25.60 303.46 299.47
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
foams [54]. Since results from foam mobility tests depends on foam the work reported in this paper.
velocity, foam quality, and permeability of the medium, the results
should only be compared to works with similar conditions. Gland et al. Data Availability
[55] developed a cationic surfactant formulation and performed
sand-pack tests at 80 ◦ C and 1740 psi. Sand-pack permeability was No data was used for the research described in the article.
estimated as 13,000 mD. For a foam quality of 80% and an injection
velocity of 43 ft/day, an apparent viscosity of ~410 cp was reported. Acknowledgements
Wang and Mohanty [32] proposed a formulation containing 500 ppm of
ethyl cellulose nanoparticles dispersed in brine along with 2.5 wt% A. Soto and A. Somoza acknowledge the Spanish Ministry of Science
non-ionic surfactant. Foam mobility experiments were performed at and Innovation and State Research Agency for financial support
100 psi and ambient temperature in a sand-pack with a high perme­ throughout project PGC2018–097342-B-I00, including European
ability (16,000 mD). Foam quality was kept at 80% and a total flow rate Regional Development Fund). A. Somoza also acknowledges Predoctoral
of 14 ft/day was applied. A promising pressure gradient larger than Financial Support (grant ref. PRE2019–089101).
100 psi was reported. However, the high surfactant concentration would
likely turn the process economically unfeasible. In a subsequent work, References
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