Article

pubs.acs.org/IECR

Investigation of Low-Density CO2 Injection for Enhanced Oil

Recovery
Seyyed Mehdi Seyyedsar,* Seyed Amir Farzaneh, and Mehran Sohrabi
Heriot-Watt University, Edinburgh EH14 4AS, U.K.
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ABSTRACT: The density of the CO2-rich phase in a reservoir would play a crucial role in the performance of an enahcned oil
recovery (EOR) scheme. Many oil reservoirs are located in deep formations; hence, they have high temperatures. Moreover, the
pressure of reservoirs decreases because of natural depletion. Under the conditions of those reservoirs, CO2 would be a low-
density gas. A series of coreflood experiments were performed to evaluate the potential of low-density CO2 EOR. The
experiments are intermittent CO2 injection, continuous tertiary and secondary CO2 injection, and water alternating CO2
injection followed by the coinjection of a surfactant and CO2. The same oil and gas were mixed to prepare live oil for all the
experiments. The initial rate of oil recovery during secondary waterflood was high, but the efficiency of the process decreased
after the breakthrough. Three pore volumes (PVs) of secondary CO2 injection resulted in the recovery of around 50% of the
initial oil in place, which was 27% higher than the oil recovered during 1 PV of water injection. It was also observed that CO2
injection can improve the recovery factor after waterflood. However, the performance of tertiary CO2 injection is reduced
because of the presence of water in pore spaces, which likely makes the oil less accessible to CO2. Waterflood after a period of
CO2 injection recovered 20% of initial oil in place mainly because of the dissolution of CO2 in the oil and the resultant oil
viscosity reduction. The impact of the rate of CO2 injection on the efficiency of oil recovery was investigated, and it appears that
the dissolution of CO2 in the oil is the main mechanism of enhanced recovery. The reduction of oil viscosity as a result of the
dissolution of CO2 in the oil as well as the low density of CO2 improved the effect of gravity drainage on oil production. In
addition, it was observed that the mechanism of solution gas drive plays an important role in the process of oil recovery. The
analysis of the physical properties of the core effluent reveals that CO2 can also improve the quality of produced oil compared to
that of the original oil in the rock. The results of this study provide experimental evidence of the potential of low-density CO2
EOR.

■ INTRODUCTION
The feasibility of CO2 injection for either light or heavy oil
immiscible.12 The mechanisms by which immiscible CO2
injection could enhance oil recovery have been investigated
recovery has been shown by various laboratory investiga- for many years. However, the impact and significance of them
tions.1−7 Several field trials have also shown a considerable have not been well-documented in the literature. For instance,
increase in oil production after CO2 injection.8−11 In light oil the mechanism of extraction of hydrocarbons by CO2 is
systems, miscibility between CO2 and the oil is usually a target, generally neglected for heavy oil reservoirs because it is
and it is often achievable by increasing reservoir pressure or
enriching the injection fluid.11 However, in the case of medium Received: January 21, 2017
or heavy oil reservoirs, the decrease in the interfacial tension Revised: March 31, 2017
(IFT) is not as significant as that in the light oil systems, and Accepted: April 20, 2017
the contact between the oil and CO 2 would remain Published: April 26, 2017

© 2017 American Chemical Society 5443 DOI: 10.1021/acs.iecr.7b00303

Ind. Eng. Chem. Res. 2017, 56, 5443−5454
Industrial & Engineering Chemistry Research
perceived as a slow process.7,13 These mechanisms include oil
viscosity reduction,6,14 oil swelling,15 IFT reduction,12 extrac-
tion of hydrocarbons,16,17 and asphaltene precipitation.18
In many of the CO2 EOR studies or field trials in the
literature, CO2 has been a relatively dense fluid, mainly a
supercritical fluid and in a handful of cases a liquid fluid.9,11
Thus, significant volumes of CO2 need to be compressed and
injected into the reservoirs when economically feasible.7,19
That, of course, is in addition to the problems stemming from
the high mobility of CO2 in porous media.20 However, many oil
reservoirs all around the world have high temperatures.21,22
Moreover, oil reservoirs usually experience a natural decline in
their pressure by beginning production. Under the conditions
of those reservoirs, CO2 would be a vapor gas with a low
density.23 CO2 injection into those reservoirs could also be a
promising process mainly for of two reasons: First, a lower CO2
density means that lower volumes of CO2 need to be
compressed, and that can make the process feasible in locations
that a large volume of CO2 is not available. Second, the costs of
compression are reduced because the injectant density is lower.
In our previous studies, it was observed that not only the rate of
CO2 dissolution and diffusion in the oil is affected by CO2
density, it also determines the impact of mechanism of
extraction on the process of oil recovery.7,13 Accordingly, it is
crucial to investigate the performance of oil recovery by low-
density CO2 injection. To accomplish this task, the same core
and fluids (e.g., oil, brine, CO2) used in our previous
experiments7,13 were used in the experiments reported in this
work to be able to compare the behavior of oil recovery at
different conditions.
An important purpose of a coreflood experiment is to
understand or predict the behavior of fluids and rocks during a
variety of field processes such as production or injection
schemes, of course, on a small scale. Although a test with a core
cannot completely mimic the complexity of processes in an
actual reservoir, the information obtained from that can be used
to predict the behavior of a reservoir. Among those advantages,
however, one critical disadvantage of a coreflood experiment is
that the trace of reservoir time cannot be seen in a coreflood
run; thus, in processes in which time-dependent phenomena
take place (e.g., diffusion), that could lead to incorrect
translation of the coreflood results. The practice of CO2
injection for enhancing oil recovery is one of the processes in
which time plays a crucial role in the performance of oil
recovery.13
In this study, the results of four coreflood experiments which
were performed at 50° C and 600 psi will be presented and
discussed. It should be mentioned that all the live fluids were
also prepared at the temperature and pressure of the
experiemnts. The first experiment is an investigation of
intermittent CO2 injection. The injection strategy is particularly
suitable for systems in which mass transfer between the
displacing and displaced fluids plays a crucial role in the
efficiency of a process. In the second experiment, the tertiary
injection of CO2 was investigated. In many reservoirs around
the world, water has been injected as the first intervention
method for improving the recovery factor.24 Therefore, it is
necessary to evaluate the efficiency of low-density CO2
injection in waterflooded porous media. The third experiment
is an investigation of secondary continuous CO2 injection. In
the fourth experiment, the performance of water and CO2
injection in an alternating manner was first investigated. Then,
the coinjection of a surfactant solution and CO2 was performed
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to further enhance oil recovery. In addition, the compositional
analysis of the core effluent and the measurements of PVT
properties of fluids were performed to identify the underlying
mechanisms of the process of oil recovery.
■ EXPERIMENTAL SETUP AND PROCEDURES
A temperature-controlled air oven was used to house all the
components of the rig other than the pumps [e.g., core-holder,
storage vessels, back-pressure regulator (BPR), pipelines, and
connections] at a constant temperature. During the experi-
ments, all the required valves could be controlled from outside
of the oven. Accordingly, that has ensured that the experiments
were performed under constant and well-controlled temper-
ature. To minimize laboratory artifacts associated with using
small core plugs, a one-piece large sandstone core with a length
of 32.1 cm was used for the experiments. The dimension and
properties of the core are given in Table 1.
Table 1. Physical Properties of the Core
property core
diameter, cm 5.13
length, cm 32.10
pore volume (PV), cm3 151.5
porosity (Φ), % 22.84
permeability to brine (K), D 2.73
The complete properties of the coreflood rig and the core
have been described elsewhere.7,13
Fluids. The same live viscous oil was used to saturate the
core in all the experiments reported here in order to highlight
the potential of CO2 injection for improving oil recovery under
the conditions of significant adverse viscosity ratios. The live oil
samples were prepared by mixing dead crude oil and
hydrocarbon gas in a heated rocking fluid recombination cell.
The dead oil was a reservoir stock-tank crude oil sample which
has a density of 0.9908 g/cm3 at 25° C and ambient pressure.
The composition of the dead oil is reported in Table 2. The
mixing of the oil and the gas was performed at a pressure and a
temperature higher than the bubble point, in order to ensure a
good mixing of them. Then the temperature of the cell was
slowly decreased to the experiment temperature, but the
pressure was still kept high to avoid degassing. Eventually, the
pressure of the cell was slowly reduced to the experiment
pressure. To measure the impact of CO2 dissolution on the oil
viscosity, another live oil sample was prepared by mixing dead
crude oil and CO2 under the conditions of the coreflood
experiments. The oil viscosities were calculated by measuring
the pressure drop through an in-line calibrated capillary tube.
The ratio of dissolved gas in the oil (GOR) samples was also
measured. Table 3 gives the measured physical properties of the
oil samples.
A synthetic brine solution with a total salinity of 10 000 ppm
was used in this study. The brine was made of 8000 ppm
sodium chloride (NaCl) and 2000 ppm calcium chloride
(CaCl2), and it was degassed before saturating the core.
Furthermore, live (methane-saturated) brine was prepared to
inject into the core prior to oil injection and CO2 injection.
Nonetheless, CO2-saturated brine was prepared at the
conditions of the experiments for injection into the core after
each period of CO2 injection. Using another calibrated capillary
tube within the setup, the viscosities of the brine samples were
measured too. The properties of the brine samples are given in
DOI: 10.1021/acs.iecr.7b00303
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Industrial & Engineering Chemistry Research Article

Table 2. Composition of Original Dead Crude Oil Table 4. Physical Properties of Brines
component Mw (g/mol) Z (mole %) temperature saturation pressure dissolved gas in GWR
(°C) (psi) brine (scm3/rcm3)
C6 86 0.09
C7 96 0.09 50 600 CH4 1.75
C8 107 0.46 50 600 CO2 15.85
C9 121 0.52
C10 134 0.94 Table 5. Properties of CO2 under the Conditions of the
C11 147 1.48 Experiments in This Study25
C12 161 2.30 density (g/cm3) viscosity (mPa·s) state
C13 175 3.13
0.082 0.017 vapor
C14 190 3.24
C15 206 3.85
C16 222 4.06
C17 237 3.53
C18 251 3.90
C19 263 3.68
C20 275 3.64
C21 291 3.35
C22 300 3.02
C23 312 3.11
C24 324 2.86
C25 337 2.62
C26+ 839 50.12
total 542 100 Figure 1. Oil recovery and DP across the core during secondary CO2
injection.
Table 4. Table 5 shows the physical properties of CO2 under
the conditions of our experiments. continuous injection. By the start of CO2 injection, it was
Procedure. The clean core was saturated with dead brine, observed that the heavy and viscous oil in the core could not be
and the permeability of the core was calculated (2.73 Darcy) by produced as fast as the injection rate. However, the oil
measuring the differential pressure (DP) across the core at production rate increased gradually until the breakthrough. At
several brine injection rates. Then, the core was flooded with 0.14 PV of injection, CO2 had reached the production end,
methane-saturated brine to avoid methane diffusion from live which resulted in oil recovery of 6.5% of the original oil in
oil into the brine in the core. Subsequently, live oil was injected place.
through the core, and irreducible water saturation (Swi) of 8% In an immiscible displacement, because the mobility of gas is
was achieved in all the experiments. After Swi was established, significantly higher than that of heavy oil in porous media, a
injection of fluids into the core was started. After each dramatic drop in the oil rate would be expected to happen after
experiment, the core was cleaned by injection of several cycles the breakthrough of the gas.26,27 However, that was not the case
of toluene and methanol in succession. It should be mentioned in this experiment, and it was noted that the oil rate reduction
that all the fluids were injected into the core from the top to its was relatively slow. The main reason for this observation
bottom. Unless otherwise stated, all the fluids have been probably was the impact of the mechanism of solution gas drive
injected at 7 cm3/h, which equals the frontal velocity of 1 ft/ as a result of CO2 dissolution in oil until the breakthrough. The
day.

■
RESULTS AND DISCUSSION
The main objective of the experiments reported here is to
evaluate the feasibility of low-density CO2 injection for oil
recovery. It will be discussed that whether the results and
observations of core-scale experiments could be translated to
actual reservoir conditions. Furthermore, the repeatability of
the experiments reported in this study is shown.
Experiment 1: Intermittent CO2 Injection. First
Continuous (Secondary) CO2 Injection. When the initial
water and oil distributions in the core were established,
continuous CO2 injection was started. Figure 1 shows the
recovery profile and DP across the core during the period of
speed of nucleation of the dissolved gas of heavy oil has an
inverse relationship with the viscosity of the oil, and also the gas
bubbles evolved throughout the oil phase are generally long-
lived in high-viscosity oils.28 After 0.3 PV of injection, oil was
recovered at a relatively constant rate until the end of
continuous injection. Figure 2 reveals the concentration of
methane in the produced gas during various stages of the
period of continuous CO2 injection. As can be seen, the
concentration of methane in the produced gas was relatively
high after the breakthrough because of relatively high oil rates.
However, the fraction of methane reduced as the oil rate
decreased. Further reduction of the fraction of methane is
attributed to the presence (dissolution) of CO2 in the produced
oil and perhaps the liberation of methane of oil in the core.

Table 3. Physical Properties of Oil Samples

temperature (°C) saturation pressure (psi) associated gas of oil GOR (scm3/rcm3) viscosity (mPa·s) oil swelling (rcm3/scm3)
28 1500 − − 277 000 −
50 600 CH4 10.60 3 530 1.035
50 600 CO2 30.63 733 1.040

5445 DOI: 10.1021/acs.iecr.7b00303

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Figure 2. Compositional analysis of produced gas during the period of Figure 3. Core pressure change during shut-in periods.
secondary CO2 injection.

The viscosity of oil recovered during the periods of CO2

injection, after complete separation of gas from oil, was
measured at 50° C, and the results were compared with the
viscosity of the original crude oil (Table 6). It is shown that oil

Table 6. Viscosity of Oil Recovered during Different Periods

of Experiment 1
viscosity
sample PV of Injection ratio (%)
dead crude oil − 100
1#1CO2#1 0.35−0.97 86 Figure 4. Incremental oil recovery during each period of intermittent
mixture of (1#2CO2#1, (1.3−1.6, 1.9−2.2, 2.5−3.1) 79 CO2 injection.
1#4CO2#1, 1#6CO2#1,
1#7CO2#1)
happened at early times of injection periods. Although CO2
dissolution in oil was dominant during halt periods, the
recovered after the breakthrough of CO2 had a notable lower viscosity difference between CO2 and oil in contact would have
viscosity than the original oil in the core. In this experiment, the been significant. The main mechanisms of oil recovery were oil
density of CO2 was relatively low. However, it appears that the viscosity reduction as a result of the dissolution of CO2 in the
mechanism of extraction of hydrocarbons by CO2 is responsible oil; gravity drainage; and, of course, viscous forces.
for the alteration of the viscosity of oil recovered after the Despite the relatively low amount of oil recovery in each
breakthrough of CO2. Another possible reason for the above- cycle of intermittent injection, Figure 5 clearly shows that the
mentioned observation could be the precipitation and
deposition of asphaltene of the oil which have been reported
in various CO2 EOR studies.18,29,30 However, several results
presented in previous investigations using the same crude oil
used in this study and under conditions similar to those of the
experiments reported here have shown that the contact of CO2
and the oil did not result in the precipation or deposition of the
asphaltene fraction of the oil in porous media.26 Therefore, it
appears that the precipitation or deposition of asphaltene would
have not been the case in our experiments.
Intermittent CO2 Injection. After the period of continuous
injection, the core was shut-in for a period of 24 h. Then, 0.3
PV of CO2 was injected into the core to improve recovery
factor. This process of halt−injection was repeated for 7 cycles. Figure 5. Cumulative oil recovery during the periods of continuous
The pressure of the core was monitored during the shut-in and intermittent CO2 injection.
periods, and it was observed that the core pressure decreased
during each of the shut-in periods (Figure 3). This observation changing of injection scheme has improved oil recovery. This
is in contrast with the observations made during the halt significant additional oil recovery was achieved mainly because
periods of the experiments where CO2 was a more dense of increasing the residence time of CO2 in a porous medium,
fluid.13 The reduction of pressure during the shut-in periods is which facilitated the dissolution of CO2 in oil.
an indication of dissolution of CO2 in the oil, and as the oil in Tertiary Waterflood. After the seventh cycle of intermittent
contact with CO2 became relatively saturated with that, the rate CO2 injection, CO2-saturated brine was injected through the
of pressure reduction decreased notably in successive cycles. core. Water advancement in the core resulted in the
The profiles of incremental oil recovery of each slug of CO2 displacement and accumulation of oil ahead of the water
injection of intermittent injection are shown in Figure 4. Before front, and an oil bank was formed. The oil bank then reached
the beginning of injection, the core pressure was increased up the outlet of the core and led to a considerable amount of oil
until the flowing pressure of the system. No oil production recovery (Figure 6). At a certain point, water reached the
5446 DOI: 10.1021/acs.iecr.7b00303
Ind. Eng. Chem. Res. 2017, 56, 5443−5454
Industrial & Engineering Chemistry Research
Figure 6. Incremental oil recovery and DP across the core during
tertiary waterflood.
production outlet, but the oil recovery continued at high water
cuts after the breakthrough. Moreover, gas production
decreased sharply when the oil bank reached the production
outlet.
Summary. Figure 7 illustrates the cumulative oil recovery
during different stages of experiment 1. The CO2 dissolution in
Figure 7. Cumulative oil recovery during different periods of
experiment 1.
the oil and the resultant effects of that on the physical
properties of oil enhanced the efficiency of oil recovery. The
increasing of the residence time of CO2 in porous media
facilitated the contact between CO2 and oil while the utilization
of gas was significantly reduced. In addition, lower-viscosity oil
could be recovered as a result of the injection of CO2. It was
observed that improving the viscosity of displacing fluid led to
the recovery of a significant fraction of oil that has been in
contact with CO2.
Experiment 2: Tertiary CO2 Injection. First (Secondary)
Waterflood. Following the procedures to establish initial oil
and water saturations, methane-saturated brine was injected
through the core. Figure 8 shows the profile of oil recovery and
DP within the core during the period of secondary waterflood.
The recovery profile is similar to waterflooding of heavy oil
systems. An early breakthrough and production of a
considerable fraction of oil at high water cuts are the main
characteristics of those systems. Hence, a significant volume of
the core remained unswept, and continuing waterflood could
not target the remaining oil.
Tertiary CO2 Injection. Figure 9 shows the profiles of oil
recovery and DP during the period of tertiary CO2 injection. A
significant fraction of the water in the core was displaced during
the period of CO2 injection. However, because of the
dissolution of CO2 in oil and water, water could not be
displaced as fast as the injection rate. The dissolution of CO2 in
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Figure 8. Oil recovery and DP across the core during secondary
waterflood.
Figure 9. Incremental oil recovery and DP across the core during
tertiary CO2 injection.
the oil, either by direct contact or by diffusing from the water
around oil, has resulted in oil viscosity reduction as well as the
swelling of oil. Consequently, oil was recovered at a relatively
constant rate until the end of the period of CO2 injection.
Despite the production of oil at a constant rate, the DP is
decreasing, which means that the viscosity of fluids contributing
to flow (mainly oil) is also decreasing. Other mechanisms such
as gravity drainage would have also contributed to oil recovery.
The composition of oil recovered during different stages of
experiment 2 was analyzed and is reported in Table 7.
Additionally, the viscosity of oil recovered by tertiary CO2
injection was measured at the temperature of the experiment
(Table 8). It is shown that the physical properties of oil have
been altered by the injection of CO2 into the core, albeit to a
small extent. These observations are mainly attributed to the
mechanisms which were also active during the injection of
dense CO2 for heavy oil recovery.7 The lower density of CO2 in
the vapor state is believed to be the main reason for the small
extent of the in situ changes of the properties of the oil.
Another reason could be due to the impact of gravity drainage,
which was more significant on oil recovery in this experiment.
Second Waterflood. After the period of tertiary CO2
injection, CO2-saturated brine was injected through the core
for a period of 1 PV of injection (Figure 10). The injected
water followed the least resistance paths of gas in the core and
then reached the production outlet. A small fraction of oil was
recovered before the breakthrough; however, the oil rate
increased sharply after the breakthrough, and oil production
continued until the end of waterflood. The compositional
analysis of the oil displaced by water confirms that the injected
water contacted the oil which was in contact with CO2.
Summary. Figure 11 shows the cumulative oil recovery
during different periods of experiment 2. The performance of
waterflood for oil recovery is a function of the viscosity ratio of
DOI: 10.1021/acs.iecr.7b00303
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Industrial & Engineering Chemistry Research Article

Table 7. Composition of Oil Recovered during Different Periods of Experiment 2

PV of ≤C12 >C12−≤C16 >C16−≤C20 >C20−≤C23 >C23−≤C29 >C29−≤C45 >C45−≤C100
sample injection (mole %) (mole %) (mole %) (mole %) (mole %) (mole %) (mole %)
2#1WF#1 0.0−0.07 12.8 22.9 28.9 12.2 12.7 8.5 2.0
2#1CO2#2 3.0−4.2 15.9 21.8 28.6 11.7 11.9 8.0 2.0
2#2WF#1 0.24−0.28 9.4 24.1 26.0 12.0 13.5 11.5 3.4

Table 8. Viscosity of Oil Recovered during Tertiary CO2 recovery. Here, the injection rate of CO2 was set at 1 cm3/h to
Injection evaluate the effects of time and rate of injection on the process
of oil recovery. Figure 12 shows the profiles of oil recovery and
sample PV of injection viscosity ratio (%)
dead crude oil − 100
2#1CO2#1 1.8−3.0 81
2#1CO2#2 3.0−4.2 83

Figure 12. Oil recovery and DP across the core during secondary CO2
injection.

Figure 10. Incremental oil recovery and DP across the core during
second Waterflood.
Figure 11. Cumulative oil recovery during different periods of
experiment 2.
the oil and water in porous media. Therefore, the sweep
efficiency of waterflood is generally poor for viscous oil
recovery. The injection of low-density CO2 after waterflood can
still enhance oil recovery mainly by mechanisms associated with
the dissolution of CO2 in the oil. It was known that the
dissolution and diffusion of CO2 is a slow process, particularly
in low-pressure systems. Therefore, time is an important factor
determining the efficiency of enhanced oil recovery by CO2
injection. The physical properties of oil can be altered by vapor
CO2. This alteration is more dominant in viscosity of produced
oil. The injection of a fluid with mobility lower than that of
CO2 can improve the sweep efficiency significantly. This is
further facilitated by the lower viscosity of the oil in porous
media because of the dissolution of CO2 in the oil.
Experiment 3: Secondary Continuous CO2 Injection.
Continuous (Secondary) CO2 Injection. A secondary injection
of CO2 followed by a period of waterflood was performed to
evaluate the potential of low-density CO2 injection for oil
DP across the core during the period of secondary injection of
CO2. It was observed that the oil in the core could not be
produced as fast as the injection rate. The relatively low rate of
injection of CO2 would have assisted the low oil rate before the
breakthrough by reducing the impact of viscous forces.
Nonetheless, for a short period of time before the break-
through, oil was produced at high rates. The early breakthrough
of CO2 demonstrates that the rate of injection does not have a
significant impact on the sweep efficiency and that the
instability in the flood front dominates the flow in the systems
of adverse viscosity ratio.
After the breakthrough, oil production continued at a
relatively constant and low rate until around 3 PVs of injection.
The main mechanism of oil recovery was the dissolution of
CO2 in the oil and the resultant oil viscosity reduction. After 3
PVs of injection, the oil rate was further decreased, which was
noticed by the rising GOR until the end of the injection of CO2
(Figure 13). The reduction of oil rate during late times of the
run was perhaps due to the lower saturation of oil in the core as
well as the reduction of the rate of diffusion of CO2 in the oil. It
should be noted that in comparison with the previous
experiments, the impact of gravity drainage on oil recovery
Figure 13. Produced GOR during secondary CO2 injection.

5448 DOI: 10.1021/acs.iecr.7b00303

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Table 9. Composition of Oil Recovered during Different Periods of Experiment 3

PV of ≤C12 >C12−≤C16 >C16−≤C20 >C20−≤C23 >C23−≤C29 >C29−≤C45 >C45−≤C100
sample injection (mole %) (mole %) (mole %) (mole %) (mole %) (mole %) (mole %)
3#1CO2#1 0.15−0.34 13.3 24.2 29.1 11.8 12.1 7.9 1.6
3#1CO2#2 1.1−1.3 13.1 24.5 29.2 11.6 12.0 7.9 1.7
3#1CO2#5 2.9−3.3 13.9 24.1 29.5 11.9 12.1 7.5 1.0
3#1WF#1 0.26−0.37 12.0 23.2 28.9 12.7 12.8 8.4 2.1

would have been higher in this test mainly because of the
significant time of the contact of oil and CO2 in the core.
The compositional analysis of oil recovered during different
stages of experiment 3 is reported in Table 9. After the
breakthrough, the composition of oil recovered by CO2
injection was remained relatively unchanged at different steps
of this run. This implies that the impact of CO2 dissolution and
gravity drainage were probably significant during the period of
CO2 injection. Moreover, the amount of free CO2 in pore
spaces could be low because of the dissolution of CO2 in the
oil. This perhaps has reduced the strength of the mechanism of
extaction of hydrocarbons by CO2. However, this does not
necessarily reflect that CO2 could not alter the physical
properties of the initial oil in the core. The composition of oil
recovered by waterflood changed slightly, reflecting that the
remaining oil in the core was relatively heavier than the oil
recovered during the previous period of CO2 injection. In
addition, the viscosity of oil recovered during the period of CO2
injection was measured, and the results, given in Table 10,
did not have a notable impact on the amount of oil produced
before the breakthrough. However, for a short period after the
breakthrough, oil was recovered with a lower rate in the
experiment in which the rate of injection was also lower. This
observation highlights the impact of solution gas drive on oil
recovery as a result of pressure rising before the breakthrough.
The higher pressure of injection fluid until the breakthrough
would have resulted in a higher amount of CO2 dissolution in
the oil. The higher pressure gradient would also enhance the
impact of viscous forces on the process of oil recovery.
Tertiary Waterflood. CO2-saturated brine was injected
through the core after the period of secondary CO2 injection.
The injected water followed the least resistance paths of CO2 in
the core, and it displaced gas toward the production outlet. A
low fraction of the remaining oil in the core was recovered until
the breakthrough (Figure 15). Oil production rate increased

Table 10. Viscosity of Oil Recovered during Secondary CO2

Injection
sample PV of injection viscosity ratio (%)
dead crude oil − 100
3#1CO2#3 1.6−1.9 90
3#1CO2#4 2.4−2.9 88

confirmed that higher-quality oil has been recovered by CO2
injection. All the viscosity measurements were performed at the
temperature that the coreflood experiment was conducted.
Effect of Rate of Injection (Time) on Performance of
Secondary CO2 Injection. Figure 14 compares the performance
of oil recovery by secondary CO2 injection in experiments 1
and 3. The rate of injection of CO2 was 7 times lower in
experiment 3. The instability in the flood front, regardless of
the rate of injection, dominated the flow until the breakthrough
time in both experiments. Hence, the rate of injection of CO2
Figure 14. Comparison of profiles of oil recovery during secondary
CO2 injection (experiment 1) and secondary low-rate CO2 injection
(experiment 3).
5449
Figure 15. Incremental oil recovery and DP across the core during
tertiary waterflood.
after the breakthrough because of the production of the oil
bank ahead of the water front. Oil was produced continuously
at high water cuts until the end of the waterflood. The relatively
low amount of oil recovery is mainly attributed to the low
saturation of the remaining oil in the core.
The results of the coreflood experiments in this study show
that the behavior of waterflood after an extended period of CO2
injection probably depends on the scheme of recovery prior to
that waterflood. For example, a distinct difference is the
production of a considerable fraction of oil before the
breakthrough by waterflood after the period of intermittent
injection while an insignificant amount of oil is recovered
before the breakthrough during waterflood after continuous
injection of CO2. The main reason for this observation would
be related to the injection scenario of CO2 before the
waterflood. CO2 during the shut-in periods could invade a
higher area of the core; therefore, the potential pore volume for
water to invade would have been higher after intermittent
injection of CO2.
Summary. Figure 16 illustrates the cumulative oil recovery
during different periods of experiment 3. The breakthrough of
CO2 was not affected by reducing the rate of injection of CO2.
The main mechanism of oil recovery was the dissolution of
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Industrial & Engineering Chemistry Research
Figure 16. Cumulative oil recovery during different periods of
experiment 3.
CO2 in the oil and the resultant oil viscosity reduction. An
advantage of low-density CO2 injection compared to dense
CO2 injection is that the mechanisms of extraction and
liberation of methane of oil are less effective. The liberation of
methane of oil by dense CO2 leads to an initial increase in the
viscosity of the oil which later is compensated by the
dissolution of CO2 in oil. However, in the case of low-density
CO2 injection, the viscosity of the oil is being reduced from the
beginning of the contact of CO2 and live oil. The performance
of tertiary waterflood after an extended period of CO2 injection
depends on the saturation of remaining oil in place as well as
the scheme of injection of CO2.
Experiment 4: Water Alternating CO2 Injection. First
(Secondary) Waterflood. The first slug of water alternating
CO2 injection was an injection of methane-saturated brine into
the core saturated with live crude oil. Following the procedures
to establish initial water and oil distributions in the core, the
injection of water into the core was started. This experiment
(experiment 4) was performed at the same conditions that the
experiment of tertiary CO2 injection (experiment 2) had been
performed. In both experiments, (methane-saturated) brine was
the first injection fluid after establishing irreducible water
saturation in the core. Figures 17 and 18 compare the profiles
Figure 17. Comparison of profiles of oil recovery during secondary
waterflood (experiment 2) and secondary waterflood (experiment 4).
of oil recovery and DP across the core, respectively, during the
period of first (secondary) waterflood in both experiments. It is
ensured that the results and also the behavior of the fluids and
the rock were repeatable in the coreflood experiments reported
in this study.
First (Tertiary) CO2 Injection. After the period of first
(secondary) waterflood, 1 PV of CO2 was injected at 1 cm3/h
through the core. Figure 19 compares the profiles of recovery of
the remaining oil in the core by tertiary injection of CO2 in
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Figure 18. Comparison of profiles of DP across the core during
secondary waterflood (experiment 2) and secondary waterflood
(experiment 4).
Figure 19. Comparison of profiles of incremental oil recovery during
tertiary CO2 injection (experiment 2) and first CO2 injection
(experiment 4).
experiments 2 and 4. The main difference in both experiments
was the rate of CO2 injection. The injection of CO2 was
continued for an almost equal period of time in both runs, as
evident in Figure 20. It should be mentioned that the difference
in the saturation of the remaining oil in the core was negligible
before the beginning of CO2 injection.
Figure 20. Comparison of performance of incremental oil recovery
during tertiary CO2 injection (experiment 2) and first CO2 injection
(experiment 4).
The results of oil recovery reflect that higher amount of oil
was recovered by a higher rate of injection of CO2 into the
core. However, in the scale of the core used in this study, the
volume of CO2 utilized in the run of high rate of injection is 6
times higher than the volume of CO2 injected at a lower rate. In
an actual reservoir, the amount of time for CO2 to contact oil
would be significantly higher; hence, a greater amount of oil can
be recovered by increasing the rate of injection of CO2. It
should be mentioned that none of the flow rates at which CO2
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Industrial & Engineering Chemistry Research
was injected into the core in these two experiments is
considered as the optimum rate of injection. Many factors,
such as availability of injection gas, injectivity of formation,
reservoir heterogeneity, and capacity of production facilities,
can affect the rate of injection of a gaseous fluid into an oil
reservoir.11,20
Water Alternating CO2 Injection. After the first period of
CO2 injection, two more cycles of water and CO2 injection
were performed to improve the recovery factor (Figure 21). A
Figure 21. Cumulative oil recovery during different periods of water
alternating CO2 injection.
significant amount of the remaining oil in the core was
recovered by (CO2-saturated) waterflood after the first period
of CO2 injection. The behavior of this period of waterflood was
notably similar to the performance of the period of second
waterflood in experiment 2. The continuation of the experi-
ment by CO2 injection after the second waterflood improved
recovery factor as well. However, the impact was not as
significant as it was during the period of first CO2 injection,
perhaps because of the lower saturation of oil in the core and
also a lower amount of oil being accessible to CO2 by water-
shielding. The performance of the third waterflood was
significantly poorer; hence, the run was terminated after only
0.5 PV of injection. The reasons for poor recovery of
waterflood could be due to the presences of established paths
of water and CO2 within the core and the low saturation of oil
in those paths of interest of water. The distributions of
saturation of the fluids in the core at the end of each slug of
injection are compared in Figure 22 in which the extent of
reshuffling of water and CO2 is noted.
It is significant that the oil was still recovered during the third
period of CO2 injection. The dissolution of CO2 in oil causes
oil swelling as well as oil viscosity reduction which would
improve the mobility of oil in porous media. The ability of CO2
Figure 22. Distribution of fluid saturation at the end of each slug of
water alternating CO2 injection.
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to drive oil toward the production outlet at this stage of the
experiment suggests that improving sweep efficiency of CO2
injection by lowering its mobility in porous media may further
enhance recovery factor from of the oil.
Coinjection of Surfactant and CO2. After the last (third)
slug of CO2 injection, the cumulative oil recovery of 57% of the
initial oil in the core was achieved, meaning that the significant
saturation of the remaining oil in place can still be a target of
EOR techniques. Although CO2 injection could still recover the
remaining oil in the core, the efficiency of this process was
relatively low. A solution to reduce the mobility of CO2 in
porous media is the combining of CO2 injection with a
surfactant solution to form in situ foam. Table 11 provides the
properties of the surfactant used in this study.
Table 11. Physical Properties of Surfactant
commercial active
name type (wt %) formula
Petrostep C1 anionic 39 (C14) sodium alpha olefin
sulfonate
Under the conditions of the coreflood experiments reported
in this paper, Emadi26 performed two coreflood experiments
using the same surfactant solution in this study. First, the clean
core was saturated with the surfactant solution, and then CO2
and surfactant were simultaneously injected through the core
(CO2 at 4.5 cm3/h and surfactant at 2.5 cm3/h). The behavior
of DP was monitored and recorded during the experiment.
After 2 total pore volumes (TPVs) of injection, it was observed
that the DP was increased at a constant rate until 6 TPVs of
injection and then remained relatively constant until the end of
the run (8.3 TPVs). The results indicated that relatively strong
and stable foam was formed during the late times of the period
of coinjection. The apparent viscosity of the foam was also
calculated by using the data of DP across the core. The core
was then prepared for the second experiment by cleaning it
with toluene and methanol injected in succession. In the second
experiment, after a period of secondary waterflood, CO2 and
the surfactant were injected simultaneously into the core. The
waterflood after 1 PV of injection resulted in the recovery of
19% of the initial oil in the core. The 6 TPVs of the coinjection
of CO2 and the surfactant (CO2 at 4.5 cm3/h and surfactant at
2.5 cm3/h) improved oil recovery by the production of 56% of
the initial oil in place during this period. The DP across the
core increased significantly before the breakthrough because of
the formation of an oil bank. The production of the oil bank
was continued until the breakthrough of CO2, which was
accompanied by the reduction of the DP within the core. Later,
the DP increased gradually almost until the late times of the
period of coinjection. Accordingly, it was concluded that in situ
formation of “CO2-foam” was the main reason for the rising DP
at late times of the run. That is, the formation of foam in the
core took place while a significantly high saturation of oil was
still in the core.
In this work, 0.1 PV of the surfactant solution was injected at
7 cm3/h into the core after the third slug of CO2 injection. This
surfactant preflush was conducted to reduce the adsorption of
the surfactant on the rock surface during the period of
coinjection of surfactant and CO2. The injected surfactant
displaced CO2 toward the production outlet, and a small
fraction of oil (less than 1% of the remaining oil in place) was
also produced during this period. Then, the coinjection of CO2
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Industrial & Engineering Chemistry Research
and surfactant was started at a total rate of 7 cm3/h (CO2 at 4.5
cm3/h and surfactant at 2.5 cm3/h). The coinjection of CO2
and surfactant was continued at a constant total rate until
around 5.8 TPVs of injection where the rates of injection (of
both fluids) were doubled and continued until 7.4 TPVs of
injection. Here, the injection was stopped and the core was shut
to charge the storage vessels with the injection fluids. After 24
h, the coinjection of surfactant and CO2 into the core was
continued but at a different total rate of injection of CO2 and
surfactant: CO2 at 11.5 cm3/h and surfactant at 2.5 cm3/h. This
run was continued at a constant rate until 2.7 TPVs of injection,
where the rate of injection of CO2 was increased to 18.5 cm3/h.
The results of the above-mentioned periods, the profile of
incremental oil recovery and the behavior of DP across the
core, are illustrated in Figures 23 and 24. Unlike the
Figure 23. Incremental oil recovery and DP across the core during the
first period of coinjection of surfactant and CO2.
Figure 24. Incremental oil recovery and DP across the core during the
second period of coinjection of surfactant and CO2.
observation made by Emadi,26 no clear sign of formation of
strong foam in the core was noted during the periods of
coinjection of CO2 and surfactant in the experiment reported
here. The cores used in both studies were taken from the same
block of rock, and their physical properties were very similar;
however, the core had been exposed to surfactant in the study
reported by Emadi26 before performing the coreflood experi-
ment with oil. Thus, the significance of adsorption of the
surfactant on the surface of rock would have been lower in that
study. However, a significant volume of surfactant was utilized
in our study, which probably eliminates the role of adsorption
in opposing the formation of foam in the core. The core in our
study was initially saturated with live (methane-saturated)
crude oil instead of dead oil in the study reported by Emadi.26
Furthermore, because of the injection of several cycles of CO2
and CO2-saturated brine, the remaining oil in the core would
have been relatively saturated with CO2. The presence of
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dissolved gas in the oil could affect the phase behavior of the oil
and the surfactant solution (i.e., optimal salinity).31,32 There-
fore, it could be a reason for no propagation of foam in the
coreflood experiment performed in our study. The presence of
gas, in particular, CO2 in oil would also reduce the IFT between
CO2 and the oil. Therefore, oil would tend to spread between
CO2 and the aqueous solution in the pores, and this can delay
the propagation speed of foam. The spreading behavior of oil
can also cause fast destabilizing of foam in porous media.33,34 In
spite of the coinjection of CO2 and surfactant into the core, the
pressure gradient within the core was lower during this run
compared to the third slug of CO2 injection. This observation
may also show that the flow paths of the fluids were different in
these two runs. In addition, the physical properties of the core
effluent, such as its color, indicated that emulsification was
significant between oil and the surfactant solution. The
emulsion scavenged the surfactant; hence, a lower amount of
surfactant was probably available for formation of foam in the
core.
The results of this study highlight the complexity of the
processes in porous media. This becomes even more
challenging in the processes in which mass transfer plays a
key role in determining the performance. It is, therefore,
important to fully understand these processes and carefully
study their underlying mechanisms prior to making decisions
on implementation of those processes in actual reservoirs.
Summary. Figure 25 illustrates the cumulative oil recovery
during different stages of experiment 4. A combination of CO2
Figure 25. Cumulative oil recovery during different periods of
experiment 4.
injection with a higher viscous fluid injection (e.g., water)
further improves the sweep efficiency in porous media. It is
believed that the remaining oil in the core after three cycles of
water and CO2 injection was mainly trapped by capillary forces.
Thus, it was aimed to reduce the saturation of oil in the core by
coinjection of CO2 and a surfactant solution. The successful
coreflood application of the coinjection of CO2 and the
surfactant solution used in this experiment has been reported in
other investigations. 26,27 However, no sign of strong
propagation of foam was observed in this study, mainly because
of the presence of dissolved gas (methane and CO2) in the
remaining oil in the core.
■
CONCLUSIONS
Four coreflood experiments were performed at various injection
strategies to evaluate the performance of low-density (vapor)
CO2 injection for oil recovery. The mechanisms involved in
these experiments were investigated and discussed. It was
shown that the coreflood experiments performed in this study
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Industrial & Engineering Chemistry Research
were repeatable. Furthermore, the compositional analysis and
the measurement of physical properties of the effluent (e.g., oil,
gas) of the coreflood experiments were performed at several
stages of the experiments. Based on the results of the
experiments reported in this work, the following conclusions
are drawn:
• In an immiscible contact, the contact of low-density CO2
and oil leads to the dissolution of CO2 in the oil and
hence the viscosity of the oil reduces.
• Low-density CO2 is capable of in situ improvement of
the physical properties (e.g., viscosity) of oil.
• In a tertiary injection of low-density CO2, the amount of
dissolution of CO2 in the water in porous media should
be considered for determining the proper amount of
CO2 for injection.
• Although time is a dominant factor in determining the
performance of oil recovery by CO2 injection, viscous
forces also have crucial impact on the speed of oil
production. Thus, increasing the rate of injection of CO2
would increase the rate of oil production.
• The presence of dissolved gas in oil can affect the
performance of coinjection of CO2 and surfactant.
Therefore, it is essential to evaluate the phase behavior
of surfactant and oil under reservoir conditions.
■
AUTHOR INFORMATION
Corresponding Author
*E-mail: ss828@hw.ac.uk.
ORCID
Seyyed Mehdi Seyyedsar: 0000-0002-4306-7374
Notes
The authors declare no competing financial interest.
■ ACKNOWLEDGMENTS
This work was carried out as a part of the Nonthermal
Enhanced Heavy Oil Recovery joint industry project (JIP) in
the Centre for Enhanced Oil Recovery and CO2 Solutions of
Institute of Petroleum Engineering at Heriot-Watt University.
The project was equally funded by Total E&P, ConocoPhillips,
CONACyT-SENER-Hidrocarburos − Mexico, Pemex, Winter-
shall, and Eni, which is gratefully acknowledged.
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