Journal of Dispersion Science and Technology

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Synergistic effect of mixed anionic and cationic

surfactant systems on the interfacial tension of
crude oil-water and enhanced oil recovery

Rashmi Kumari, Abhijit Kakati, R. Nagarajan & Jitendra S. Sangwai

To cite this article: Rashmi Kumari, Abhijit Kakati, R. Nagarajan & Jitendra S. Sangwai (2019)
Synergistic effect of mixed anionic and cationic surfactant systems on the interfacial tension of
crude oil-water and enhanced oil recovery, Journal of Dispersion Science and Technology, 40:7,
969-981, DOI: 10.1080/01932691.2018.1489280

To link to this article: https://doi.org/10.1080/01932691.2018.1489280

Published online: 08 Oct 2018.

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JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY
2019, VOL. 40, NO. 7, 969–981
https://doi.org/10.1080/01932691.2018.1489280

ORIGINAL ARTICLE

Synergistic effect of mixed anionic and cationic surfactant systems on the

interfacial tension of crude oil-water and enhanced oil recovery
Rashmi Kumaria,b
, Abhijit Kakatib
, R. Nagarajana, and Jitendra S. Sangwaib
a
Department of Chemical Engineering, Indian Institute of Technology Madras, Chennai, India; bEnhanced Oil Recovery Laboratory, Petroleum
Engineering Program, Department of Ocean Engineering, Indian Institute of Technology Madras, Chennai, India

ABSTRACT ARTICLE HISTORY

Surfactant based enhanced oil recovery (EOR) is an interesting area of research for several petrol- Received 25 April 2018
eum researchers. In the present work, individual and mixed systems of anionic and cationic surfac- Accepted 10 June 2018
tants consisting of sodium dodecyl sulphate (SDS) and cetyltrimethylammonium bromide (CTAB)
KEYWORD
in different molar ratios were tested for their synergistic effect on the crude oil-water interfacial
Critical micellar
tension (IFT) and enhanced oil recovery performance. The combination of these two surfactant concentration; EOR;
systems showed a higher surface activity as compared to individual surfactants. The effect of interfacial tension; mixed
mixed surfactant systems on the IFT and critical micellar concentration (CMC) is strongly depends surfactant; synergism
on molar ratios of the two surfactant. Much lower CMC values were observed in case of mixed
surfactant systems prepared at different molar ratios as compared to individual surfactant systems.
The lowest CMC value was found when the molar concentration of SDS was higher than the
CTAB. When the individual and mixed surfacant systems were tested for EOR performance through
flooding experiments, higher ultimate oil recovery was obtained from mixed surfactant flooding
compared to individual surfactants. Combination of SDS and CTAB or probably other anionic-cat-
ionic surfactants show synergism with substantial ability to reduce crude oil water IFT and can be
a promising EOR method.
GRAPHICAL ABSTRACT

Introduction
International Energy Outlook (2016) shows that the global
primary energy demand will increase by 48% by the end of
2040. Even though the non-fossil fuels are expected to grow
faster but the fossil fuel will still be expected to account
about 78% of the energy resources in 2040. The increasing
demand of fossil fuels is compelling upstream oil companies
to explore new oil reserves, but it seems to involve huge
capital expenditure because most of the new reserves are
expected to occur in challenging conditions, such as deep-

CONTACT Jitendra S. Sangwai jitendrasangwai@iitm.ac.in Enhanced Oil Recovery Laboratory, Petroleum Engineering Program, Department of Ocean
Engineering, Indian Institute of Technology Madras, Chennai, India.

Equal contribution
ß 2018 Informa UK Limited, trading as Taylor & Francis Group
970 R. KUMARI ET AL.
Table 1. Properties of the crude oil used in this study.
Properties Values
Specific gravity 0.8286
API gravity 39.30
Viscosity @ 40oC (cSt) 2.70
Pour point (oC) 30
Sulphur (wt. %) 0.12
Acid number (mg KOH) 0.12
water and under high pressure and high temperature
(HPHT) conditions. Matured oil reservoirs still expected to
contain more than 50% of the original oil in place which
can be produced using novel enhanced oil recovery (EOR)
methods.[1] To increase recovery efficiency of these matured
oilfields, different industries practice different EOR methods
involving injection of different chemicals, e.g., surfactant,
alkali, polymer, gas, etc. EOR with surfactant injection (sur-
factant-EOR) is pursued as a means of increasing oil pro-
duction in many of the major oilfields in the world.[2–7]
Surfactant-EOR method is gaining interest of oil producers
in improving oil recovery as the surfactant used in EOR has
the potential to recover more oil where other EOR methods
are failed. Although, this method has a great potential to
improve oil recovery, more research is necessary to under-
stand the effect of various surfacants and their synergism to
increase the oil production from these reservoirs.
The main function of injecting surfactant into the reser-
voirs is to reduce the interfacial tension (IFT) between crude
oil and water. However, the mechanism of surfactant-EOR
can be explained based upon two different functions: 1.
Reduction in IFT, and 2. Wettability alteration. Reduction in
oil-water IFT increases the capillary number which interns
reduces the residual oil saturation.[8] Stegemeier[2] shows
that in order to reduce the residual oil saturation by half,
the capillary number must be increased by 1000 times. The
wettability alteration using surfactant is more important and
could be achieved more in carbonate reservoirs since they
show a more oil-wet behaviour. The IFT can be affected by
many parameters, such as the type of surfactant and its con-
centration, oil composition and its properties, salinity, pres-
sure, temperature conditions, etc.[9] Surfactants used in EOR
applications can be classified depending on the ionic nature
of their headgroup in an aqueous solution, and these are,
anionic, cationic, nonionic and zwitterionic. Anionic surfac-
tants are very effective in lowering IFT and have low
adsorption on reservoir rock.[10] Various authors have inves-
tigated different type of anionic surfactants for EOR applica-
tions, such as alcohol propoxylate sulphate[11, 12], internal
olefin sulfonates.[13, 14] Nonionic surfactants, such as alco-
hols, phenols, ethers, esters or amides, etc., are used in EOR
as co-surfactants.[15] Cationic surfactants are not as widely
used as anionic and non-ionic surfactants because they are
expensive. However, they can improve spontaneous imbibi-
tion rate of water into oil-wet carbonate reservoirs by shift-
ing the rock wettability towards water-wet state.[16] The
structure of the surfactant should be tailored in accordance
to the reservoir type to ensure that the surfactant are opti-
mal for the reservoir condition.[17]
Table 2. Details on the chemicals used in this work.
Chemical CAS Number Purity (%)
Manufacturer
Sodium 7647-14-5  99 Merck, Mumbai, India
chloride
SDS 151-21-3 85 Sisco Research Laboratory(SRL),
Mumbai, India
CTAB 57-09-0 99 Sigma Aldrich
PAM 9003-05-8  80 Triveni Global Pvt. Ltd., Chennai, India

As stated by the manufacturer.
Table 3. Properties of PAM used for polymer flood.
Product ZETAG
Appearance Off-white granular solid
Bulk density (g/cc) Approx. 0.7
pH of 1% solution at 25oC 6.0-9.0
Anionic charge Very low
Apparent viscosity (cP) at 25oC at concentration (wt %)
0.25 0.50
0.5 200
1.0 1100
Surfactant mixtures are known to have more pronounced
interfacial properties in comparison to their individual com-
ponents. The synergistic effect of surfactant mixtures on
interfacial properties, micelle formation, rheology, foaming,
phase behavior, etc., has been reported earlier by various
authors.[18–27] However, studies on the synergistic effect of
surfactant mixtures for EOR are very limited. Li et al.[28]
designed a lipophilic surfactant by mixing a hydrophilic
anionic (nonylphenyl ethoxylate carboxylate) and cationic
(quaternary ammonium) surfactant capable of producing
lower critical micellar concentration (CMC), IFT values and
high oil solubilization. From coreflood experiments, they
found that the surfactant mixtures were useful for tertiary
oil recovery from low salinity reservoirs. El-Batanoney
et al.[29] tested the synergistic effect of surfactants by blend-
ing four different fatty acid amides with dodecyl benzene
sulfonic acid. The IFT between aqueous solution with differ-
ent surfactant blends and Badri crude oil were tested. One
of the surfactant blend which was found to produce lowest
IFT value was used for displacement experiments and a sig-
nificant recovery was obtained. Gogoi[30] studied the mix-
ture of didodecyldimethylammonium bromide (cationic
surfactant) and sodium lignosulfonate (anionic surfactant)
for oil recovery from Naharkotiya oil field. Jia et al.[31]
studied the effect of combining a cationic ionic liquid (N-
dodecyl-N-methylpyrrolidinium bromide) and an anionic
surfactant sodium dodecyl sulfate on IFT and oil recovery
performance. Apart from IFT studies, investigations have
also been done to understand the synergistic effect of mixed
surfactants on the wettability of rock forming mineral surfa-
ces.[32, 33] Also, sodium dodecyl sulphate (SDS) surfactant
has been studied widely in combination with nano-particles
by various researchers in order to enhance the surface activ-
ity.[34] The synergism between SDS and a cationic surfactant,
cetyltrimethylammonium bromide CTAB for air-water has
been studied by few authors and observed to have enhanced
surface activity.[35, 36] The use of SDS þ CTAB for EOR and
its effect on crude oil-water IFT have not been reported pre-
viously, although it was reported for air-water surface. To
the best of our knowledge, mixed surfactant systems have

Figure 1. (a) SEM image of silica sand sample used in this study; (b) XRD pattern of the silica sand used in this study.
not been widely used until currently for the commercial
application in the oil industry and therefore it is necessary
to conduct more research from a practical EOR point
of view.
Present work investigates the synergistic effect of combin-
ing an anionic surfactant, SDS, and a cationic surfactant,
CTAB, on the oil recovery efficiency of a paraffinic crude
oil. The work reports the results on IFT measurements
between Bombay High crude oil and aqueous surfactant sol-
utions containing SDS, CTAB and their mixtures in different
molar ratios, such as SDS þ CTAB (0.3:0.7; 0.5:0.5; 0.3:0.7).
Laboratory based core-flood experiments were conducted on
crude oil saturated sand-pack at high temperature to see the
oil recovery performance of different surfactant combina-
tions and to compare with pure surfactant systems.
JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY 971
Experimental
Materials
Crude oil
Crude oil used in this study is a stock tank crude oil from
Bombay-high oilfield, India. The crude oil is provided by
Chennai Petroleum Cooperation Limited (CPCL). The prop-
erties of the crude oil are listed in Table 1.
Chemicals
The purity, grade and manufacturer of the chemicals used
in this work are presented in Table 2. The properties of the
polyacrylamide (PAM) used for flooding experiments are
listed in Table 3.
972 R. KUMARI ET AL.
Figure 2. Schematic of experimental set-up for surfactant-EOR flooding experiments.
Porous media
Clean silica sand was used to prepare the sand-pack porous
media for flooding experiments. The SEM image of sand
particles in Figure 1(a) shows the size and morphology. The
majority of the particles are in the range of 0.4 - 0.8 mm.
The mineralogical composition of the sand is determined by
X-ray diffraction. The X-ray diffraction pattern of the sand
particles [Figure 1(b)] where peaks of 2h are obtained at
20.919, 26.753, 27.651, 36.626, 39.468, 50.293, 68.339, and
73.574 indicates that it is composed primarily of quartz
(96 wt. %) with a small amount of feldspar (0.0353%).[37–39]
Experimental setup and procedure
IFT measurements
The IFT measurements between surfactant solutions and
crude oil were measured using Wilhelmy plate method. A
dynamic contact angle tensiometer (Dataphysics DCAT 11,
Germany) was used for this purpose. The instrument consists
of a microbalance to measure the force required by the
Wilhelmy plate (Dataphysics PT-11) to break down the liquid
film at the oil-water interface. SCATVR software was used for
height positioning of the sample vessel and automatic return-
ing of IFT values. The instrument has an accuracy of
±0.01 mN.m1. The sample temperature was measured with a
built-in temperature sensor which has an accuracy of ±0.1 K.
Temperature control was done using a water bath (Brookfield
TC 650). Before each measurement, the Wilhelmy plate was
properly cleaned by dipping in clean alkane solvents and dis-
tilled water followed by drying of the plate in a blue flame.
To prepare various surfactant solutions, surfactants are meas-
ured using LC GC RADWAG AS/X 220 analytical balance
(RADWAG Wagi Elektroniczne, Poland; repeatabili-
ty, ± 0.1 mg; readability 0.1 mg) with ±0.00004 mass fraction
of uncertainty. A more detailed procedure regarding the IFT
measurement is reported in our previous work.[40, 41]
Preparation of sand-pack
All flooding experiments were conducted using a sand-pack.
The sand-pack was prepared by filling the sand-pack reactor
(bulk volume: 649 cm3) with clean and dried silica sand with
gradual addition of distilled water. The sand column was pre-
pared compactly by ramping the sand thoroughly. The
amount of water required in making the sand-pack is consid-
ered as the pore volume (PV) assuming the sand -pack to be
100% saturated with water. The porosity (%) of the sand-
pack is calculated as the ratio of bulk volume to pore volume.
Preparation of injection fluids
Five different surfactant solutions were prepared, i.e., SDS,
CTAB, and SDS þ CTAB (0.3:0.7, 0.5:0.5, 0.7:0.3) using stock
solutions in distilled water by stirring vigorously at 1000 rpm
for 1 h. The same solutions were used for IFT studies followed
by EOR studies. The PAM solution of 5000 ppm concentration
was peppered using powdered PAM in distilled water with vig-
orous and constant stirring at 1000 rpm using mechanical stir-
rer (Model:121/D, Remi Elektrorechnik Ltd, Vasai,
Maharashtra, India) at 1000 rpm for 24 h. Brine solution was
prepared using NaCl of 30,000 ppm concentration.
EOR flooding experiments
The flooding experiments were performed using a setup rep-
resented in Figure 2. The flooding experiments were con-
ducted under a high temperature (353.15 K) which was
maintained by circulating hot water in the jacket surround-
ing the sand-pack inside the reactor. The hot water circula-
tion was done using a water bath (Brookfield TC-650AP
with operating temperature range of 20  C to þ200  C). A
syringe pump (Teledyne ISCO 500 D with maximum cap-
acity 508.7 ml) was used for injection of fluid stored in fluid
accumulator into the sand-pack.
Sand-pack saturation. After the sand-pack was prepared, it
was pre-flushed with sufficient PV of NaCl brine (30000 ppm)

which replace the distilled water from the pores to simulate the
saline condition of oil reservoirs. During all the experiments,
fluids were injected at a constant flow rate (5 ml/min). The
pressure differential across the sand-pack (between the inlet
and outlet) is recorded after every 0.1 PV of the fluid collected
at the outlet. The absolute permeability (k) of the sand-pack
was calculated using Darcy’s law during this pre-flush. After
pre-flushing with brine, crude oil was injected into the brine
saturated pack. Sufficient PV of crude oil was injected into the
pack until the production of water was stopped to establish ini-
tial or irreducible water saturation and initial crude oil satur-
ation. The volume of water came out of the pack is equal to
the volume of crude oil retained inside the pack which is called
as the original oil in place (OOIP). The initial oil saturation
(Soi) and water saturation (Swi) is calculated as,
OOIP
Soi ¼
100% [1]
PV
PV OOIP
Swi ¼
100% [2]
PV
Effective permeability to oil (ko) in presence of water was
also calculated during crude oil injection. The viscosities of
the injection fluids required for Darcy’s calculations were
measured with a rotational viscometer (Brookfield DV2TLV,
spindle: SC4-18, measuring range: 0.2–30,000 cP).
After establishing the initial fluid (oil and water) satura-
tions, the sand-pack was aged for a long time (approximately
for 8-12 hours) at the experimental temperature to attain equi-
librium between the sand particles and injected fluids.
Secondary oil recovery (waterflood). Since any EOR process
always targets the residual oil left after secondary recovery
(waterflooding), therefore a secondary recovery was initiated to
mimic the waterflood in the oil reservoir. To establish a
residual oil saturation after waterflood (and before injecting
the surfactant solutions), almost 2 PV of brine was injected
into the aged sand-pack until the water production becomes
nearly 100%. The residual oil saturation (Sor) is calculated as:
OOIPvolume of oil produced
Sor ¼
100% [3]
PV
Enhanced oil recovery (surfactant-EOR). Individual EOR
experiments have been performed for various surfactant sol-
utions containing the individual and mixtures of anionic
and cationic surfactant in the molar ratio of SDS þ CTAB
(0.3:0.7; 0.5:0.5; 0.7:0.3). After injecting 2 PV of brine, 0.5
PV of surfactant solution was injected in each experimental
case for surfactant-EOR studies. The production stream
from outlet of the sand-pack was collected in graduated cyl-
inders. The volumes of produced oil and water collected
were noted at regular intervals. This values are used to cal-
culate the recovery factor as a function of injected fluid vol-
ume. At the end of surfactant flooding, a polymer flood was
performed for all the individual experiments, where a slug
of 0.5 PV of PAM is injected. After polymer injection, the
sand-pack was flooded with 2 PV of chase brine to recover
as much oil as possible and mimic the actual reservoir oil
recovery practices.
JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY 973
Results and discussion
Present study has been carried out to investigate the syner-
gism between different types of surfactants in mixtures for
enhanced oil recovery. The synergism is expected to results
in the utilization of low amount surfactant used for a par-
ticular application, which in turn reduces both cost and
environmental impact. Initially, the results on IFT measure-
ments between crude oil and different surfactant aqueous
systems (individual and mixed) used in this study have been
discussed. Subsequently, the results on the surfactant-EOR
studies performed with five different surfactant systems
using light paraffinic crude oil from Bombay high oilfield of
India have been presented.
IFT studies
This investigation sheds light on the effect of different indi-
vidual and mixed surfactant systems, such as SDS, CTAB and
combinations of SDS and CTAB in different molar ratios on
the IFT of crude oil-water system. The results of IFT experi-
ments are presented as IFT vs. molar concentration of surfac-
tants in Figure 3(a–e). IFT of the crude oil- pure water
system is found to be 20.60 mN/m. From these results, it can
be observed that the interfacial tension initially reduces with
an increase in surfactant concentration and reaches almost a
flat plateau. This trend was observed for all five surfactant
systems studied in this work. The concentration at which IFT
becomes constant is considered as the critical micellar con-
centration (CMC). CMC is also interchangeably referred in
various literatures as critical aggregation concentration.[42–44]
Although the surface tension is ideally to be constant when
the surfactant concentration exceeds the CMC value, but in
case of the surfactant-oil system studied in the work, the sur-
face tension was not observed to be perfectly constant after
the CMC. However, a very insignificant change was observed
in the IFT when the concentration exceeded CMC. After the
CMC values, the slopes of the IFT graphs is observed to be
very small and insignificant which could be considered almost
constant. When surfactants added to an aqueous phase, the
surfactant monomer moves towards the interface and forms a
monolayer reducing the interfacial tension. After a certain
concentration value, the surfactant monomer starts forming
closed aggregates known as micelles with their hydrophobic
tail in an oil phase while the hydrophilic head in water. This
phenomenon results in the reduction of IFT, the minimum
IFT corresponds to the CMC of the surfactant. It indicates
the point at which surface active properties are at an opti-
mum condition. In Figure 3(a–e), the CMC is determined as
the concentration corresponding to the intersection point or
breakpoint of the trend lines following the two distinct trends
of IFT values with surfactant concentrations. It can be
observed that before attaining CMC, the IFT decreases grad-
ually with increase in surfactant concentration in case of indi-
vidual surfactants [Figure 3(a, b)]; whereas for mixed
surfactant systems, a rapid decline in IFT has been observed
with increase in surfactant concentration [Figure 3(c–e)]. In
case of single surfactant system, the IFT of crude oil-water
system at CMC is higher for SDS (2.91 mN/m) than CTAB
974 R. KUMARI ET AL.

Figure 3. IFT between crude oil-water containing individual and mixed surfactant systems: (a) only SDS; (b) only CTAB; (c) SDS þ CTAB (0.3: 0.7); (d) SDS þ CTAB
(0.5: 0.5); (e) SDS þ CTAB (0.7:0.3). Numbers in bracket shows molar ratios.

(0.12 mN/m). In case of mixed surfactant systems, a low IFT

Figure 4. Comparison of CMC values for different surfactant systems. Numbers
in bracket shows molar ratios.
was obtained. The IFT of crude oil-water at CMC in case
mixed surfactant systems are found to be 1.3 mN/m for
SDS þ CTAB (0.3:0.7); 0.19 mN/m for SDS þ CTAB (0.5:0.5)
and 5.021 mN/m SDS þ CTAB (0.7:0.3). The minimum IFT
at CMC was observed in case of equal molar ratios of the
surfactants used. Even though, the mixed surfactant systems
have shown a low IFT, these are slightly higher than the pure
CTAB case but lower than the SDS case. Although the IFT of
crude oil-water is low in case of pure CTAB system; but
CTAB could not be used alone due to its cost and adsorption
tendency onto the rock surface.[45]
Figure 4 compares the CMC values of five surfactant sys-
tems studied in this work. It has been observed that the

Figure 5. Schematic of the surfactant aggregation mechanism at crude oil-water interface for mixed (cationic þ anionic) and individual surfactant systems.
Table 4. Petrophysical properties of the sand-pack used for various EOR
experiments.
Permeability (mD)
Sand-pack
number Porosity (%) Swi (%) Soi (%) kw (Sw ¼1)
1 34.51 43.30 56.70 544
2 34.82 42.48 57.52 438
3 32.36 41.90 58.10 396
4 33.90 40.00 60.00 472
5 34.67 48.89 51.11 504
CMC values for mixed surfactant systems are much lower
than the individual single surfactants. SDS has a relatively
higher CMC value (4.6 mM) as compared to the CMC value
obtained for CTAB (1.4 mM). It can be seen that there is a
decrease in the values of CMC of the order 102 to 103
when these surfactants are used in combinations. The
decrease in CMC value is more (of the order 103) in both
cases where one of the ionic surfactant is higher in concen-
tration, i.e., SDS þ CTAB (0.3: 0.7) or SDS þ CTAB (0.7:
0.3). The reduction in CMC of equimolar ionic surfactant
system, i.e., SDS þ CTAB (0.5: 0.5) is in order of 102.
When two or more substances produces a combined effect
more than the sum of their individual effects then it is
known to exhibit a synergism. It is known for a long time
that anionic-cationic binary surfactant systems exhibit strong
synergism in both reducing surface tension and mixed
micelle formation.[46] For a given surfactant system, good
IFT reduction is shown only when surfactants have an
appreciable, but limited, solubility in both oil and aqueous
phase. Interfacial properties will be changed with the add-
ition of counterions. Head groups of ionic surfactants with
the same charge produces electrostatic repulsion which acts
as the main contributor to increase the free energy of
micelle formation.[47] Thus, if a surfactant with oppositely
charged head group is incorporated, the micelle aggregation
number is expected to increase.[48] Due to this strong inter-
action of molecules, IFT also expected to reduce to lower
JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY 975
values. Thus, when oppositely charged SDS and CTAB are
mixed, it enhanced the formation of worm like micelles
because SDS reduces the surface potential via charge neu-
ko (Swi) tralization and increases the ionic strength by virtue of
184 released counterions. Figure 5 shows the schematic on the
169 mechanism of the aggregation of surfactant molecules at the
192
167 crude oil-water interface for single and mixed surfactant sys-
189 tems. Experimental study shows that mixtures of surfactants
with unequal tail lengths promotes formation of micelle.[49]
According to Parekh et al.[50] when the tail length of the
two surfactant differs then more vesicle formation occurs in
case of surfactant mixture which is rich in shorter tailed sur-
factants. Since SDS has a shorter tail length than CTAB,
therefore we have observed lowest CMC value for the sur-
factant system where SDS concentration is higher than
CTAB, i.e., SDS þ CTAB (0.7: 0.3). Again, the tendency of
micelle formation not only depends on tail lengths but also
on the relative concentration of the two surfactants.[36] Tah
et al.[35] observed formation of micelle by CTAB/SDS cata-
nioic mixtures in an aqueous solution at unequal molar ratio
for both higher CTAB and SDS case. In this study we
observed a CMC values for both higher SDS and higher
CTAB case compared to the equimolar concentration case.
Lower IFT was also been observed by Jia et al.[31] for the
crude oil and mixed surfactants with higher SDS concentra-
tion. Again, according to Shang et al.,[51] for equimolar mix-
tures of cationic and anionic surfactants, when the tail
length differs for each surfactant in the mixture, then pre-
cipitation takes place. The precipitation may affect the effi-
ciency of micellar formation as in case of equimolar
concentration; which is in-line with our observation from
Figure 4. In any surfactant precipitation process, the pres-
ence of micelles can itself decrease the tendency of precipita-
tion. In this study, the surfactant concentration used for
enhanced oil recovery is above micellar concentration (or
aggregation concentration). However, as a preventive
976 R. KUMARI ET AL.
Figure 6. Cumulative oil recovery and water cut vs. pore volume (PV) injected for: (a) only SDS; (b) only CTAB; (c) SDS þ CTAB (0.3: 0.7); (d) SDS þ CTAB (0.5: 0.5);
(e) SDS þ CTAB (0.7 þ 0.3) at 353.15 K. Sequence of flooding is as follows: 2 PV brine flooding, 0.5 PV surfactant/mixed surfactant flooding, 0.5 PV brine and 2PV
chase brine flooding.
measure non-ionic surfactants could be added to cationic-
anionic surfactant systems to prevent precipitation.[52]
Further studies are necessary to investigate in detail the pre-
cipitation and adsorption of mixed surfactant systems onto
rock surface.
Results of surfactant-EOR experiments
This study investigates enhanced oil recovery performance
of the individual and combinations of anionic and cationic
mixed surfactant systems through laboratory-based flooding
or displacement experiments conducted on a sand-pack
under simulated reservoir condition of a typical petroleum
reservoir (see Figure 2 for experimental set-up). The total
surfactant concentration of the surfactant slug is three times
of the concentration of the respective CMC values, i.e., SDS:
13.3 mM; CTAB: 4.2 mM; SDS þ CTAB (0.7:0.3): 0.075 mM;
SDS þ CTAB (0.5:0.5): 0.012 mM and SDS þ CTAB (0.3:0.7):
0.021 mM. The petrophysical properties of the various sand-
packs used in EOR experiments are reported in Table 4. The
results of the surfactant-EOR flooding experiments are pre-
sented in Figure 6(a–e) as cumulative oil recovery vs.
injected PV for each surfactant system. The associated pres-
sure drop is also plotted, while the relevant properties of the
sand-pack (such as, Soi,/, k, etc.) corresponding each surfac-
tant-flooding case has been mentioned in Table 4. Table 5
gives details on the Soi, Sor and additional oil recovery in
various surfactant-EOR cases investigated. As mentioned in
the experimental procedure, once the sand-pack has been
saturated with crude oil at an initial conditions of Soi and
 JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY 977

recovery (% of OOIP)
Cumulative oil

65.59
69.46
84.95
79.50
90.09
Total additional

(% of OOIP)
oil recover

14.65
18.31
24.85
24.05
39.21
Chase brine
Additional oil recovery (% of OOIP)

7.24
10.23
6.08
16.97
26.96
flood
over brine flood
Polymer

6.22
6.38
18.38
6.63
10.70
flood

Figure 7. Comparison of cumulative oil recovery from injection of different sur-

factant systems.
Surfactant
flood

Swi (as in Table 4), brine flood (2 PV), followed by surfac-

1.18
1.69
0.38
0.45
1.56

tant-EOR (0.5 PV), then polymer flood (0.5 PV), and finally
chase water flood (2 PV) have been employed to understand
initial brine flood or

the oil recovery potential of various surfactant combinations

Secondary recover
Oil recovery from

(% of OOIP)

mentioned in Table 5.
50.94
51.15
60.11
55.45
50.87

Figure 6(a–e) portrays that, during the initial waterflood-

ing (secondary water flood), the water cut has increased
almost rapidly (prompt breakthrough) and reached the max-
imum point (almost 100%) in short duration in almost all
the cases of surfactant -EOR. Subsequently, surfactant flood-
Chase brine
flood (2PV)
19.51
17.57
8.56
12.29
5.07

ing has been employed followed by a polymer injection. The

water cut has reduced slightly (by about 2–5%) during the
surfactant flooding, but at the end of surfactant flooding it
increased again and reached almost 100%. When polymer
flood (0.5 PV)
Polymer

flood was started, water cut found to be decreased from

23.62
23.45
12.02
22.48
18.84
Sor (% of PV) after
Table 5. Summary of results of the different flooding experiments performed in this work.

about 100% to about 30 to 60%. At the onset of the chase

brine flood, the low water cut (in the range of 30 to 60%)
from previous polymer flood remained active for some time,
flood (0.5PV)

but after a certain point, the water cut again increased and
Surfactant

27.14
27.12
22.49
26.45
24.31

reached its maximum level (100%).

Figure 6(a–e) shows that the oil recovery first increases
directly with injected brine volume during brine flood (0.5
PV), but after some time the oil recovery decreased to
Brine flood

27.81
28.10
22.71
26.73
25.11
(2PV)

almost about 0%, while the water cut increases to 100%.

This indicate the end of brine flood (water flood) perform-
ance and the need to initiate surfactant-EOR flood. When
(% of PV)

surfactant flood (0.5 PV) was employed, the oil recovery did
56.70
57.52
56.92
60.00
51.11
Soi

not improve much, i.e., it was in the range of 0.5% to 2%

of the OOIP. This may be due to the fact that only 0.5 PV
surfactant solution has been injected, which did not pushed
SDS þ CTAB (0.3: 0.7)
SDS þ CTAB (0.5: 0.5)
SDS þ CTAB (0.7: 0.3)

the oil out of the sand-pack. During this process, the surfac-
Surfactant

tant is expected to get adsorbed at the sand/crude oil/water

system

interfaces, which subsequently affect (reduces) the IFT

between them. After the end of surfactant injection, polymer
CTAB
SDS

flood (0.5PV) has been injected. During the polymer flood,

the oil recovery was increased in the range of about 6% to
Sand pack

18% of the OOIP (Table 5). Again, only 0.5 PV of polymer

number

flood has been injected, which acts like a piston effect for
subsequent chase water flood. The significant increase in the
1
2
3
4
5
978 R. KUMARI ET AL.
oil recovery increment is observed during the chase brine
flood. The oil recovery during the chase brine flood has
been found to be in the range of 6–27% of the OOIP, how-
ever after some time, the recovery started to decrease and
finally reaches 0%, while the water cut reaches to 100% (see
Figure 6 and Table 5). During the chase water flood, it was
found that only 7% to 10% of the oil has been recovered in
case of individual SDS-EOR and CTAB-EOR, respectively;
however, in the case of mixed surfactant systems, around
6% - 27% crude oil was recovered. It has been observed that
the injected surfactant can affect the crude oil recovery till
the chase brine flooding, therefore, in order to compare the
effect of different surfactant systems on crude oil recovery,
the total additional oil recoveries and cumulative oil recov-
eries have to be considered as reported in Table 5.
The total additional oil recoveries in the case of individ-
ual SDS-EOR and CTAB-EOR are observed to be 14.65%
and 18.31%, respectively, while in the case of anionic-cat-
ionic mixed surfactant combinations (SDS þ CTAB), it was
found to be 24.85%, 24.05% and 39.21% for the molar ratios
of 0.3:0.7, 0.5:0.5 and 0.7:0.3 (SDS þ CTAB), respectively. As
shown in Table 5, the cumulative oil recovery for SDS and
CTAB was found to be 65.59% and 69.46%, respectively. It
can be seen that CTAB performs better than SDS but it is
Figure 8. Pressure drop during flooding for different surfactant-EOR cases.
Figure 9. Schematic of the oil recovery mechanism by individual and mixed surfactant systems.
not widely used in the industry due to its cost. As compared
to the cumulative oil recoveries of individual surfactants,
anionic-cationic mixed surfactant (SDS þ CTAB) systems
have shown much higher cumulative oil recovery, i.e.,
84.95%, 79.50% and 90.09% for the molar ratios of 0.3:0.7,
0.5:0.5 and 0.7:0.3, respectively. These results are analogous
to the IFT and CMC results obtained above. As discussed
earlier, in case of only SDS-EOR, the CMC value was high-
est (4.6 mM) and also shown higher IFT values as compared
to the other surfactant systems used in this study, which
resulted in lowest cumulative oil recovery of 65.59% of
OOIP. The highest cumulative oil recovery (90.09% of
OOIP) was observed for SDS þ CTAB surfactant-EOR case
for the molar ratio of 0.7: 0.3, for which the CMC value was
found to be lowest (0.004 mM) among all the surfactant sys-
tems used in this study. Figure 7 shows a comparison of the
cumulative oil recoveries from individual and the mixed sur-
factant-EOR processes.
Figure 8 represents the pressure drop across the sand-
pack as a function of total or cumulative injected fluid vol-
ume (in terms of PV). It can be inferred that the pressure
drop across the sand-pack during waterflooding (0–2 PV)
did not vary considerably and was in the range of
0.15–0.22 MPa. The pressure drop even did not vary much
during surfactant flooding (2–2.5 PV) and observed to be in
the same range as of waterflooding. However, during the
polymer flood (2.5–3 PV) injection, the pressure drop was
found to be increase gradually and was in the range of
0.22–0.47 MPa. It was also found to be increasing continu-
ously till the beginning of extended chase brine flood in the
range of 0.47–0.61 MPa, but after certain PV of chase brine
injection, it was decreased gradually.
Certain surfactants can reduce the oil-water IFT to very
low level. Synthesis of such kind of surfactant is a sophisti-
cated and expensive process. However, the ultra-low IFT are
difficult to obtain with every surfactant system. The surfac-
tants used in our study are cost effective. Although CTAB is
slightly expensive, the outcome of core-flooding experiments
show that the best recovery performance could be achieved
in the case when CTAB concentration is much lower in
mixed surfactant system. However, we believe that the IFT
values for mixed surfactant cases studied in this work are
fairly low to help in crude oil mobilization. Esmaeilzadeh

et al.[53] studied the effect of SDS and CTAB concentration
on the oil-water IFT using heptane as the oil phase.
However, the observed IFT values are quite higher than the
IFT values observed in present study. This is due the differ-
ence in the nature of oils used in their study as compared to
that of the present study. Although, the SDS did not able to
reduce the IFT as effective as CTAB, but the IFT was
observed to be significantly low when used in combinations.
Again, CTAB surfactant normally tends to adsorb on silicate
mineral surface. However, the maximum enhanced oil
recovery in this study was observed in the case where the
CTAB concentration was fairly lower than the concentration
of SDS which reduces the surfactant adsorption on the sand
surface. This happens when the concentration of CTAB is
below CMC as CTAB forms monolayer. Above CMC, the
CTAB forms a bilayer on the rock surface with hydrophilic
head groups pointing towards aqueous phase which makes
the solid surface water-wet.[54] However, studies on the
adsorption of surfactant on rock surface will be carried out
in future to know more about the adsorption behavior. As
observed in this study, the mixed surfactant systems con-
taining SDS þ CTAB along with polyacrylamide as a poly-
mer flood agent have been used for coreflood experiments.
This combination has been found to give enhanced oil
recovery based on laboratory scale studies. However, other
polymer systems along with the mixed surfactant systems
have not been investigated in this work and will be done as
part of future work. Also the outcome of EOR of any such
combinations will also depend on the various other reservoir
and crude oil properties.
With addition of surfactant to oil-water system the mole-
cules of surfactant get adsorbed to the interface of the two
immiscible fluids and reducing the IFT as well the rigidity
of the interface. This phenomenon helps in deformation of
the trapped residual oil ganglia in the pore spaces of the
rock.[55, 56] It is well-known that the displacement efficiency
in the EOR is related to capillary number Nc. The capillary
number influences the residual oil saturation. The residual
oil trapped in the reservoir pore structure could be displaced
when the value of Nc increases up to 103 to 102. An
effective way to enhance the Nc is by reducing the crude oil/
water IFT and improving the mobility of displacement liquid.
Researchers have shown that the IFT must be less than
102 mN/m if the residual oil is to be mobilized.[57] From the
IFT studies carried out in this work, it is known that the com-
bination of anionic and cationic mixed surfactants shows an
IFT values of order 102 to 103 mN/m. The low IFT is prob-
ably helping in increasing the capillary number thus improv-
ing the crude oil recovery. The schematic of the possible oil
recovery process is shown in the Figure 9. It is suggested that
an oil droplet get stuck in the pore spaces of the sand grains
of the rock because its movement is restricted by smaller pore
throat and also due to high interfacial tension, it stick to the
rock surface. When surfactant or mixed surfactants are intro-
duced into the reservoir, the surfactant molecules are expected
to get aggregated at the crude oil-water interface which
reduces the IFT. The anionic and cationic mixed surfactant
systems cause very low IFT tension, which interns results in
JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY 979
the breakdown of the crude oil droplet to form microemul-
sions and distortion of its shape, so that it can pass through
the smaller pore throats as shown in Figure 9.
SDS and other anionic surfactants have been studied for
enhanced oil recovery application by various researchers and
also used in many oilfield applications.[34, 53, 58–60] Although
the application of surfactant has been proven to be an effective
enhanced oil recovery technique but an obvious question that
always arise is the environmental impact. Environmental
impact is one of the most important aspect that is always
given importance in oil and gas industry. In enhanced oil
recovery operations, precaution has always been taken so that
the injected chemicals doesn’t contaminate the shallow water
bodies. The chemicals have been injected deep into the reser-
voirs which are back produced with the produced water from
the oil wells along with oil. The produced water in most cases
is injected back into the reservoir and proper treatment has
been done in case of its reuse for oilfield operations.
Conclusion
In this work, synergistic effect of an anionic surfactant, SDS
and a cationic surfactant, CTAB on the crude oil-water IFT
and EOR performance has been studied. The following con-
clusions can be drawn from this study:
1. Combination of anionic (SDS) and cationic surfactant
(CTAB) proved to have a better surface activity in com-
parison to individual surfactants (SDS or CTAB).
2. The critical micellar concentration (CMC) is signifi-
cantly low for anionic-cationic mixed surfactant systems
for crude oil-water. The lowest CMC value was found
when the molar concentration of SDS was higher than
the CTAB.
3. The IFT could be reduced by addition of even small
amount of cationic surfactant like CTAB to an anionic
surfactant like SDS.
4. The oil recovery performance of anionic-cationic mixed
surfactant flooding is significantly higher in comparison
to each type of individual surfactant flooding. A higher
oil recovery was observed in case where the anionic sur-
factant (SDS) has higher concentration in the mixed
surfactant slug than the cationic (CTAB) surfactant.
5. Lower CMC for mixed surfactant systems implies that a
lower amount of surfactant is required for EOR applica-
tion when used in a combination.
Acknowledgement
The authors would like to acknowledge Chennai Petroleum Corp. Ltd.
(CPCL) for providing crude oil sample for this study.
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