Download as pdf or txt
Download as pdf or txt
You are on page 1of 10

126 Journal of the Japan Petroleum Institute, 62, (3), 126-135 (2019)

[Regular Paper]

Evaluation of Nanoparticle-stabilized Emulsion Flooding:


Glass-micromodel Experimental Study

Amin PAJOUHANDEH †1),†2)* , Mahin SCHAFFIE†1), and Mohammad RANJBAR†1)


†1)
Dept. of Petroleum Engineering, Shahid Bahonar University of Kerman, Kerman, Islamic Republic Blvd., 7618868366, IRAN
†2)
Abdal Industrial Project Management Co. (MAPSA), #5, Emdad Gharbi Str., Sheykhbahai N., Molasadra, Tehran 1993764638, IRAN

(Received October 16, 2018)

Emulsion flooding is a promising technique for enhanced recovery of the residual oil that cannot be recovered
through waterflooding processes. Visual micromodels are powerful tools for examining the mechanisms of oil
recovery from porous media at the pore level. A glass micromodel was used to investigate the effects of polymer
and different industrial nanomaterials on emulsion viscosity, stability and recovery factor of crude oil. The used
micromodel has uniform pore throats and grains. Experiments showed that injection of nanoparticle-stabilized
water-in-oil emulsions is an effective enhanced oil recovery method. Ultimate oil recovery was greater using
nanoparticle-stabilized emulsion/water than water/nanoparticle-stabilized emulsion/water, and the efficiency of
nanoparticle-stabilized emulsion/polymer/water also achieved greater recovery. Image analysis showed that the
ultimate recovery factor was increased from 33.99 % using water flooding to 63.28 % using nanoparticle-stabilized
emulsion/polymer/water flooding. The results of this study are helpful for the mechanistic understanding of
enhanced oil recovery projects.

Keywords
Water-in-oil emulsion, Nanoparticle, Emulsion stability, Viscosity, Micromodel, EOR

1. Introduction waterflooding, because the crude oil mobility is much


lower than the water mobility, as defined by the ratio of
Crude oil consumption is projected to increase year the effective permeability to viscosity of the fluid).
after year due to two factors: higher population and the Consequently, water breaks through quickly, so the
increasing demand in developing countries. Supplying water cut increases.
this increase in world crude oil demand will require the (2) Reservoir pore blockage.
mobilization of trapped oil. Typically, only one-fifth (3) Channeling of injected water into the heterogeneous
to one-third of the original oil deposit is recovered reservoir results in low sweep efficiency in the displace-
during primary production, but a number of EOR ment of crude oil.
(Enhanced Oil Recovery) processes can be used to Solutions to these problems include increasing the
obtain this trapped oil1)∼4). The feasibility of these viscosity of water or use of another driving fluid that
methods for field applications is closely related to the will not channel through the oil. Surfactant and nano-
flow mechanisms and porous properties in the porous fluid flooding are more efficient than waterflooding, but
medium at the microscopic level5). Approaches to have problems such as high cost and poor control of
increase the amount of oil extracted from the porous mobility. In contrast, emulsion flooding solves many
medium include decreasing the interfacial tension or of the problems and is one of the most efficient
increasing the shear viscosity of the driving fluid6). enhanced oil recovery methods. Emulsion flooding is
Waterflooding of a reservoir is a typical method used in less expensive, and achieves ultra-low interfacial ten-
the petroleum industry to increase the amount of oil sion and higher viscosity than surfactant flooding9).
recovered from a subterranean formation. However, Emulsion injection into the reservoir causes the emul-
waterflooding has various associated problems includ- sion to enter the thief zones, so that the oil bank is shifted
ing the following7),8): by a piston-like displacement10). This process occurs
(1) Poor sweep efficiency, especially for heavy oil due to the high viscosity of the emulsion and the low
interfacial tension between the emulsion and the crude
DOI: doi.org/10.1627/jpi.62.126
oil.

To whom correspondence should be addressed. Emulsions consist of the stable dispersion (droplets)

E-mail: a.pajouhandeh@gmail.com of one liquid in another immiscible liquid. Emulsions

J. Jpn. Petrol. Inst., Vol. 62, No. 3, 2019


127

can be used to lower the interfacial tension, reduce oil using 2-D glass micromodels. Micromodels are trans-
viscosity and control the mobility ratio, and may parent artificial models of porous media that can be
contain hydrocarbons, water, surfactant, cosurfactant used to observe fluid flow through porous media22).
(alcohol), and solid particles. Typically, emulsions are Micromodel flooding results can provide better inter-
divided into two groups, water-in-oil and oil-in-water pretations of flow transport during different injection
emulsions. Water-in-oil emulsions consist of water schemes in reservoirs. The first study employing a
droplets in a continuous oil phase. Water-in-oil emul- visual approach to investigate microscopic mechanisms
sions have been used in various EOR projects due to the of fluid behavior in porous media was conducted in
high viscosity and ultra-low interfacial tension. This 195223) and etched glass network was introduced24)
type of emulsion improves the mobility ratio by based on the photo etching technique25). Micromodels
increasing the viscosity of the displacing fluid11). Oil- have many applications in various areas such as EOR
in-water emulsions consist of oil droplets in a continu- processes (water flooding, water-alternating-gas flood-
ous water phase. This type of emulsion has lower vis- ing, polymer flooding, surfactant flooding, surfactant
cosity than crude oil, and can be used to enhance the foam flooding, alkaline flooding, alkaline-surfactant
production of oil from a subterranean reservoir. flooding, alkaline-surfactant-polymer flooding, surfac-
The most important features of emulsions are their tant-alkaline-polymer flooding, water-alternating-
stability and rheology12). Oil-in-water and water-in-oil solvent flooding, simultaneous water-alternating-solvent
emulsions can be stabilized by the presence of agents flooding, microbial EOR, etc.), imbibition, drainage,
(surfactants and solid particles) at the interfaces that breakthrough time, mass transfer, scaling, asphaltene
delay the spontaneous tendency of the liquids (water deposition, gravity drainage, heterogeneity, interfacial
and oil) to separate. Such agents are most commonly tension, wettability, capillary pressure, multiple contact
molecules containing both polar and non-polar chemi- miscibility, fluids interactions, etc.26)∼28).
cal groups in their structure. The presence of surfac- The advantages of emulsion flooding in the enhanced
tant in emulsions reduces the interfacial tension oil recovery process were investigated in 196629). Three
between the trapped oil and displacing fluid and stabi- separate injection phases of microemulsion, polymer,
lizes the resultant emulsion13). Heavy oils commonly and water was injected into the Chateaurenard field
contain large quantities of asphaltenes, resins and naph- (France) as a pilot test. After two months of injection,
thenic acid that act as emulsifiers. Among these com- the oil production rate increased from 20 to 75 bpd30).
ponents, asphaltene generates more stable emulsions. The viscosity of emulsions varies with the hydro-
Solid-stabilized emulsions were first proposed in 1907 phobicity of the nanoparticles31). Also, the relative
by Pickering. Such emulsions have many advantages, viscosity of solid stabilized water-in-oil emulsions varies
and are widely used in the pharmaceutical and cosmetics with the solid concentration32). Investigation of the
industries, but rarely in petroleum industries (including application of nanoparticle-stabilized emulsions to
the EOR process). Solid particles (or nanoparticles in enhanced oil recovery indicated that the apparent vis-
the petroleum industry) may also be added to the con- cosity of water-in-oil emulsion decreased with increased
tinuous phase prior to emulsification to further stabilize salinity15). Study of the effects of Aerosil R7200,
water-in-oil and oil-in-water emulsions. These nano- Aerosil R972 and the mixture of Aerosil R7200 and
particles are adsorbed on the oil-water interface to form R972 on the rheological properties of nanoparticle sta-
a rigid monolayer on the surface of the droplet, resulting bilized emulsion showed that the viscosity of emulsions
in higher stability. This type of emulsion can be trans- decreased with higher Aerosil R972 concentration in
ported over greater distances than emulsions without oil-in-water emulsions33). Study of the rheological
solid particles14),15). The stability of emulsions con- properties and stability of water-in-oil emulsions stabi-
taining nanoparticles has been extensively studied16)∼18). lized by Aerosil R972 and Cloisite 20A indicated that
The rheological behavior of emulsions is the key the viscosity and droplet size of water-in-oil emulsions
characteristic in the successful design of an emulsion are influenced by the amount and type of nanoparticles,
flooding project. Rheological properties of emulsions volume of water fraction and aging time of emul-
and solid-stabilized emulsions are affected by many sion34),35).
parameters such as temperature, dispersed phase frac- However, very few studies have investigated the
tion, average droplet size, droplet size distribution, con- effects of emulsion and nanoparticle-stabilized emulsion
tinuous phase viscosity, nature and concentration of the on oil recovery and micromodel flooding. Most
emulsifying agents, solid concentration, conditions of researchers have used surfactant-stabilized emulsions
mixing, stirring time, mixing devices, aging time, shear but emulsion stabilized by surfactant is unstable at high
rate, pressure, etc.19)∼21). temperatures and high salinity, and has higher mobility
Reliable predictions of performance and hydrocarbon that results in lower system recovery4).
recovery are essential for planned implementation of The present study investigated the rheological prop-
emulsion flooding. Such estimates can be obtained erties of water-in-oil emulsions stabilized by nano-

J. Jpn. Petrol. Inst., Vol. 62, No. 3, 2019


128

particles in the absence of molecular surfactant. One bulk water phase and a bulk oil phase, separately. If
of the main objectives was to assess water-in-oil emul- the drops readily dispersed in the water phase and re-
sion flooding, and to better understand the impact of mained intact in the oil phase, the emulsion was the oil-
emulsion and nanoparticles on oil recovery and viscous in-water type and if the opposite the water-in-oil type.
fingering. Therefore, the ultimate goal of this study is 2. 3. Stability
to enhance the sweep efficiency of conventional emul- Emulsion stability was determined by the bottle test
sion flooding containing nanoparticles by the alternating method. Prepared emulsions were stored at 70 °C in
injection of emulsion and polymer. Viscosity mea- an oven. The volume of separated water was mea-
surements were carried out, and the effects of some sured.
important parameters such as the volume fraction of 2. 4. Droplet Size Distribution
water, type of solid particles, and solid concentration on Droplet size distributions of stabilized and non-
the viscosity of water-in-oil emulsions were investigated. stabilized water-in-oil emulsions were determined by a
Finally, the emulsion flooding process was visualized Laser Particle Sizer (ANALYSETTE 22, Fritsch, Idar-
utilizing the two-dimensional glass-etched micromodel. Oberstein, Germany).
2. 5. Viscosity Measurements
2. Experimental Section The viscosity of water, dyed water, crude oil, water-
in-oil emulsions (stabilized and non-stabilized) and
2. 1. Materials polymer were determined by steady shear measure-
All experiments were carried out using crude oil (de- ments using a Brookfield DV-III Ultra Programmable
gassed crude oil with free water). The API gravity of rheometer (Brookfield, Middleboro, MA, USA). This
the crude oil was 28.7°. Deionized water was used to rheometer has concentric cylinder geometry and is con-
make emulsions. The viscosity, density, and pH of the trolled by Rheocalc V3.2 software. In addition to the
deionized water at room temperature were 1.01 (cP), viscosity measurements, microscopic observations of
0.9978 (g/cm3) and 6.32, respectively. The viscosity the resulting emulsion were conducted using a polar-
of dyed water at room temperature was 1.06 (cP). ized light microscope (Eclipse TE2000-U, Nikon,
Two industrially used nanoparticles, NP-I (Cloisite Tokyo, Japan).
20A, Southern Clay Products, Gonzales, TX, USA) and 2. 6. Displacement Tests
NP-II (Aerosil R972, Degussa, Hanau-Wolfgang, The displacement tests were carried out at room tem-
Germany) were employed. NP-I is natural montmoril- perature and under atmospheric conditions. The
lonite modified with a quaternary ammonium salt. etched glass micromodel was used, as shown in Fig. 1.
NP-II is fumed silica, treated with DDS (dimethyl- Here, the black dots represent sand grains, and the
dichlorosilane). Both nanoparticles are hydrophobic. white areas represents the flow channels. Figure 2
The particle-oil-water contact angle (​θow) of NP-I and demonstrates the macroscopic and microscopic images
NP-II are 92° and 114°, respectively. Conventional of the water (in blue) saturated micromodel. The pore
hydrolyzed polyacrylamide (HPAM), trade name of
FLOPAAM 3630S (SNF Floerger, Andrézieux, France)
with molecular weight of 20 million D and 30 % hydro-
lysis was used.
2. 2. Emulsion Preparations
Nanoparticles were added to the crude oil and soni-
cated with an ultrasonic laboratory processor (Up200H,
Hielscher, Teltow, Germany) for one hour to disperse Fig. 1 2-D Image of the Micromodel Pattern (not to scale)
aggregates. The amplitude and frequency of the ultra-
sonic treatment were 90 % (234 μm) and 0.8 (the de-
vice irradiates the sample at intervals of 0.8 sec ON and
0.2 sec OFF), respectively. The nanoparticle concen-
tration in the dispersion was 0.02, 0.05 and 0.1 by wt%.
Interfacial tension (IFT) between water and crude oil
was determined by Kruss k12. Subsequently, deion-
ized water was added to the system and dispersed with
a mechanical overhead stirrer (RW20 Digital, IKA,
Staufen, Germany). The emulsions were prepared
with three different water volume fractions (i.e., 20, 50,
80 vol%). Finally, the type of emulsion was deter-
mined using the drop test method and the microscope.
In the drop test, drops of the emulsion were added to a Fig. 2 Image of Water Saturated Micromodel

J. Jpn. Petrol. Inst., Vol. 62, No. 3, 2019


129

structure of the micromodel is symmetrical. water-in-oil emulsions. The particle-oil-water contact


Parameters of the glass micromodel are shown in angles (θ ow) of NP-I and NP-II are greater than 90°.
Table 1. A Nikon digital camera, syringe pump Figure 3 illustrates the effect of added nanoparticles
(Fusion syringe pump, Chemyx, Missouri, USA), and on the IFT between crude oil and water. Nanoparticles
microscope (YF100, Nikon, Tokyo) are the major com- added to the crude oil decreased the IFT between crude
ponents of the experimental apparatus. Initially, the oil and water from 21.63 to 18.2 mN/m with 0.1 wt%
micromodel was saturated with deionized water colored NP-I added to crude oil. NP-I decreased the IFT more
with methylene blue (Merck, Darmstadt, Germany), for than NP-II because the contact angle of NP-I is almost
easy identification in the images provided by the cam- neutral (particle-oil-water contact angle about 90°).
era. Then, a drainage process was performed using The hydrophobic part of the nanoparticles was located
crude oil until water residual saturation was reached. in the oil phase and the hydrophilic part in the water
Seven scenarios were used; additional information is phase. Consequently, these added nanoparticles were
given in Table 2. Before each experiment, the glass adsorbed at the interface between water and oil, and re-
micromodel was cleaned with sequential injection of duced the IFT37),38). Therefore, these nanoparticles are
distilled water, acetone, toluene and hydrochloric acid important in the emulsion formation process. The
(15 v/v%), and finally heated in an oven at 100 °C for at type of emulsion was determined by the drop test and
least one hour. Equation (1) which presents the effi- analyzing the photomicrographs. Figure 4 shows that
ciency consequences for oil recovery improvement the water phase was present as dispersed spherical
based on the measurements of the displacement test36): droplets, which proves that the emulsions were the
water-in-oil type. The drop test showed that the emul-
Soi − Sof
RF = × 100 (1) sion was water-in-oil, because the drops readily dispersed
Soi
in the oil phase and remained as drops in the water
where RF is the recovery factor (%), Soi is the initial oil phase.
saturation (%) and Sof is the final oil saturation (%). 3. 2. Emulsion Stability
Emulsion stability was assessed by the bottle test
3. Results and Discussion method. In this method, the extent of phase separation
with time was monitored. NP-I and NP-II form water-
3. 1. Emulsion Preparation in-oil emulsions because these particles are hydro-
Nanoparticles contained in an emulsion will be pref- phobic particles. The bottle test showed that the emul-
erentially wetted by one of the phases (water or oil) sions with added NP-I or NP-II were more stable than
more than the other phase. Nanoparticles with particle- solid-free emulsion, because the nanoparticles formed
oil-water contact angle (θow) less than 90° are water-wet
particles and stabilize oil-in-water emulsions, whereas
nanoparticles with particle-oil-water contact angle (θow)
greater than 90° are oil-wet particles and stabilize

Table 1 Glass Micromodel Characteristics

Parameter Value
Length [cm] 10
Width [cm] 3
Depth [cm] 0.01
Porosity [%] 38.96
Pore volume [cm3] 0.11688
Contact angle [°] 28 Fig. 3 IFT between Water and Crude Oil

Table 2 Investigated Scenarios

Scenario No. First step Second step Third step


1 Water - -
2 Water Emulsion Water
3 Water Nanoparticle-stabilized emulsion Water
4 Emulsion Water -
5 Nanoparticle-stabilized emulsion Water -
6 Emulsion Polymer Water
7 Nanoparticle-stabilized emulsion Polymer Water

J. Jpn. Petrol. Inst., Vol. 62, No. 3, 2019


130

rigid structures at the interfaces that can sterically Emulsions containing nanoparticles (NP-I and NP-II)
inhibit the coalescence of emulsion droplets. were more stable than the emulsions without nano-
Furthermore, the stability of solid-free and nano- particles. Therefore, the emulsion stability was
particle-stabilized emulsions decreased with higher increased by higher nanoparticle concentration. The
water volume fraction because repulsion between the adsorbed nanoparticle layer at the oil-water interface is
droplets decreased, which can intensify coalescence and not rigid at low concentrations of nanoparticles, and the
Ostwald ripening. The Young-Laplace equation (Eq. droplets were easily deformed. The adsorbed nano-
(2)) has proved this result39): particle layer at the interfaces is rigid at higher nano-

( (
1 1 particle concentrations, so the emulsion stability in-
∆P12 = ∆P1 − ∆P2 = 2γ ow − (2) creased.
r1 r2
The results showed the stability of nanoparticle stabi-
where ∆P12 is the difference in internal pressure between lized emulsion depended on the particle-oil-water con-
the droplets and γow is the interfacial tension. This tact angle (θow) value. Emulsions stabilized with NP-
equation reveals that the pressure is greater inside II were more stable than emulsions stabilized with NP-I
smaller than larger droplets. Therefore, larger water because the contact angle of NP-II is greater than that
droplet diameter associated with higher water volume of NP-I. Figure 6 shows that the separation of water
fraction decreased the emulsion stability. phase was slower in emulsion stabilized with NP-II than
Figure 5 indicates the bottle test result for water-in- in emulsion stabilized with NP-I.
oil emulsion with water volume fraction of 80 %.

Fig. 6●Percentage of Water Separation in Nanoparticle Stabilized


Fig. 4●Microscope Images of Emulsions with Water Volume Water-in-oil Emulsion with Nanoparticle Concentration of
Fraction of 50 % 0.1 wt% and Water Volume Fraction of 80 %

Fig. 5 Bottle Test Results for Water-in-oil Emulsions with Water Volume Fraction of 80 %

J. Jpn. Petrol. Inst., Vol. 62, No. 3, 2019


131

Fig. 7●Microscope Images of the Effects of Nanoparticles on Water-


in-oil Emulsions at Water Volume Fraction of 20 % (a:
without nanoparticle, b: 0.1 wt% NP-II)

Fig. 8●Droplet Size Distribution of Water-in-oil Emulsions Fig. 9 Rheological Behavior of the Crude Oil and Polymer
Containing 20 % Water Volume Fraction

fluids is independent of the shear rate. In general,


3. 3. Droplet Size Distribution crude oils with API degrees higher than 20 behave as
Water volume fraction, intensity of agitation, charac- Newtonian fluids, whereas heavy crude oils with API
teristics of the agitator, presence or absence of solids, degrees lower than 20 show non-Newtonian behaviors
and solid concentration all affect the diameter of the (shear thinning behaviors)40)∼42). Crude oil viscosity
formed emulsion droplets. Figure 7 displays typical is a function of temperature. The effect of temperature
photomicrographs (100×) of water-in-oil emulsions on crude oil viscosity can be estimated with the
illustrating the effect of nanoparticles on the droplet Arrhenius equation, which is defined by19):
diameter of emulsions containing 20 % water volume Ea
© = Ae RT (3)
fraction. The mean droplet diameter of emulsion de-
creased with higher nanoparticle concentration. Added where A is the frequency factor, E a is the activation
nanoparticles are adsorbed onto the water-oil interface, energy (J/mol), R is the gas constant (8.314 J/mol.K), T
then the surface energy of the system is reduced, so the is the temperature (K) and © is the crude oil viscosity.
established emulsion droplet becomes smaller. Figure 9b shows the relationship between the experi-
The droplet diameter distributions of solid-free and mental data and the Arrhenius equation. The degree
nanoparticle-stabilized water-in-oil emulsions contain- of fit, as given by the R2 value of 0.9858, showed that
ing 20 % water volume fraction are illustrated in Fig. 8. changes in viscosity with temperature were well
In the presence of nanoparticles, the distribution is described by the Arrhenius equation.
shifted towards smaller droplet size, in agreement with 3. 4. 2. Polymer
the microscopic images (Fig. 7). In other words, The concentration of polymer used in this experiment
emulsion droplet size distribution had a narrower range was 500 ppm. Figure 9a shows the rheological be-
with higher nanoparticles concentration. Large drop- havior of polymer at 20 °C. The polymer had non-
let size distribution centered on around 3 μm was Newtonian behavior, because higher shear rate resulted
obtained for nanoparticle-stabilized emulsion prepared in lower viscosity.
with 0.1 wt% NP-II, and about 9 μm for non-solid sta- 3. 4. 3. Water-in-oil Emulsions
bilized emulsion. The viscosity measurements were carried out imme-
3. 4. Viscosity Measurements diately at 20 °C. Figure 10 plots the viscosity of
3. 4. 1. Crude Oil water-in-oil emulsions against the water volume fraction.
Figure 9a represents the effect of shear rate on crude All values of water volume fraction affected the viscos-
oil viscosity at 20 °C. Crude oil shows Newtonian ity of water-in-oil emulsions. Therefore, the viscosity
behavior at 20 °C, because the viscosity of Newtonian of water-in-oil emulsion was increased by higher water

J. Jpn. Petrol. Inst., Vol. 62, No. 3, 2019


132

Fig. 12 Waterflooding Process

Fig. 10●Effect of Water Volume Fraction on the Viscosity of Water-


in-oil Emulsions at Different Nanoparticle Concentrations

Fig. 11●Micromodel of Crude Oil and Irreducible Water Saturation


(a: macroscopic image of the micromodel at the end of pri-
mary drainage of water, b: microscopic image of the micro-
model)

volume fraction and higher nanoparticle concentration.


The droplet size of emulsions decreased with the addi-
tion of nanoparticles (Fig. 7), so that the viscosity of
the emulsion increased. In fact, the number of drop-
lets increases by decreasing the droplet size, so the
droplets are closer together and the emulsion becomes
more rigid. However, the effect of water volume frac-
tion is greater than that of the nanoparticle concentra-
tion. Emulsion with water volume fraction of 80 %
stabilized by 0.1 wt% NP-II had the highest viscosity.
For this reason, such an emulsion is a good candidate
for emulsion flooding, because as viscosity increases,
both the capillary number and consequently the recov-
ery factor increase. Consequently, nanoparticle con-
tent in water-in-oil emulsion is dominant in determining 13.1: first scenario, 13.2: second scenario, 13.3 third scenario, 13.4:
its behavior. fourth scenario, 13.5: fifth scenario, 13.6: sixth scenario.
3. 5. Micromodel Flood Tests
Fig. 13●Micromodels after Each Scenario
A series of micromodel flood tests were carried out
to evaluate the enhancement of oil recovery using emul-
sion and nanoparticle-stabilized emulsion in porous because of the water films surrounding the grains. In
media. In addition, the effect of flooding on break- this image, liquid flowed from right to left. The con-
through and viscous fingering were investigated. tact angle of 28° proves that the glass micromodel is
Water, emulsion (with water volume fraction of 80 %), water-wet.
nanoparticle-stabilized emulsion (with water volume Figure 12 shows the four stages of the waterflooding
fraction of 80 % stabilized by 0.1 wt% NP-II) and poly- process. Figure 13.1 shows the macroscopic and
mer (500 ppm Flopaam 3630S) were injected into the microscopic images of the micromodel after the first
micromodel with fixed flow rate of 0.01 mL/min. scenario (waterflooding). Figure 12 and Fig. 13.1
Wettability of the porous medium is fundamental to indicate that during waterflooding, oil was displaced by
d e t e r m i n i n g t h e f l u i d f l ow s i n t h a t m e d i u m . the corner filament flow of water rather than by piston-
Figure 11a shows a magnified image of the micromodel like displacement. The rate of oil displacement was
at the end of primary drainage of water (blue color). strongly reduced following breakthrough of the main
Figure 11b shows that the micromodel is water-wet, fingers in waterflooding, because the mobility of the

J. Jpn. Petrol. Inst., Vol. 62, No. 3, 2019


133

a: beginning of polymer injection, b: end of polymer injection, c: be-


ginning of water injection, d: end of nanoparticle-stabilized emulsion/
polymer/water flooding.

Fig. 15●Macroscopic Images of the Nanoparticle-stabilized


Fig. 14 IFT between Crude Oil and Emulsion
Emulsion/Polymer/Water Flooding Process

displacing fluid (water) was higher than that of the dis-


placed fluid (crude oil). The calculated RF at the end
of this step was obtained by Eq. (1) as 33.99 %, which
indicates the inefficiency of waterflooding. Viscous
fingering was the dominant displacement mechanism in
this process.
Figure 13.2 shows the fluid distribution in the micro- Fig. 16 Micromodel after the Seventh Scenario
model after the second scenario, with the blue and black
colors representing water and oil (crude oil and emul-
sion), respectively. Figure 13.2 demonstrates the re- and crude oil. Lower IFT results in higher capillary
covery of additional oil by emulsion injection after the number and increased RF.
waterflooding stage. Comparison of Figs. 13.1 and Figure 13.6 shows the macroscopic and microscopic
13.2 indicates oil was displaced during emulsion flood- images of the micromodel after the sixth scenario.
ing by piston-like displacement rather than corner fila- Figure 13.6 shows that oil was recovered more effi-
ment flow of water. The RF value was 47.50 %, which ciently by co-injection of emulsion with polymer than
confirms the improvement achieved by injection of only emulsion, because oil was displaced by piston-like
emulsion into the micromodel. displacement. The RF value was 60.24 %.
Figure 13.3 shows the fluid distribution in the micro- Figure 15 shows the four stages of the nanoparticle-
model at the end of the third scenario. Comparison of stabilized emulsion/polymer/water flooding process.
Figs. 13.2 and 13.3 show that the nanoparticle- Figure 16 shows macroscopic and microscopic images
stabilized emulsion increases breakthrough time, and of the final state of nanoparticle-stabilized emulsion/
consequently increases oil recovery, as the added polymer/water flooding. Nanoparticle-stabilized
nanoparticles increase the viscosity and shear thinning emulsion/polymer/water flooding led to a very high
effect of the emulsion. The shear thinning fluid flood- microscopic efficiency, because the mobility of the
ing achieves more oil recovery than waterflooding and polymer and nanoparticle-stabilized emulsion was lower
solid-free emulsion flooding. than that of crude oil. Nanoparticle-stabilized emul-
Figure 13.4 shows the results of the fourth scenario. sions have higher viscosity (as mentioned before) and
The pore volume occupied by oil decreased compared significantly reduce the interfacial tension between
with waterflooding after injection of emulsion and trapped oil and displacing fluid (interfacial tension
water. The RF value was 45.31 %, which indicates between emulsion and oil is very low at about 0.1 mN/m)
that this process is more efficient than water flooding. which stabilizes the interface against coalescence, once
Figure 13.5 shows the micromodel network after formed. These emulsions tend to block the big chan-
injection of nanoparticle-stabilized emulsion containing nels and so force the displacing fluid to flow through
0.1 wt% NP-II in the fifth scenario. The oil was dis- the unswept regions, which increases the overall sweep,
placed with little fingering effect, because the viscosity leading to overall increase in oil recovery. However,
of the nanoparticle-stabilized emulsion was much higher the pore volume occupied by oil was decreased signifi-
than that of the crude oil and solid-free emulsion, as cantly after the last stage compared with other stages.
well as the ultra-low IFT of the emulsion flooding sys- Table 3 presents the results of the image analysis of
tem at the interface of oil-water. Figure 14 illustrates the glass micromodel. The displacement tests were
the interfacial tension between emulsion and crude oil. carried out three times and the quantitative results
Figure 3 shows the final IFT. Added nanoparticles reported are the average values obtained from the three
decrease the IFT between the solid-stabilized emulsion replication experiments. Waterflooding recovered

J. Jpn. Petrol. Inst., Vol. 62, No. 3, 2019


134

Table 3 Results of Image Analysis of the Glass Micromodel with added nanoparticles further enhanced oil recovery,
Scenario No. RF [%] (average) Standard deviation because the nanoparticles increased the viscosity
and stability of emulsions. The high viscosity of
1 33.99 3.25
2 47.50 1.20
nanoparticle-stabilized emulsions modified the mobility
3 49.58 1.16 ratio during flooding. The micromodel experiments
4 45.31 0.86 showed that nanoparticle-stabilized emulsion/polymer/
5 56.94 0.25 water flooding reduced viscous fingering and increased
6 60.24 0.78 breakthrough time to optimize improved oil recovery.
7 63.28 0.28

Nomenclatures

approximately 34 % of the initial oil in place, and solid A : frequency factor [-]
Ea : activation energy [J/mol]
stabilized-emulsion/polymer/water flooding recovered RF : recovery factor [%]
an additional 30 % of the initial oil in place. Table 3 R2 : regression correlation coefficient [-]
demonstrates that the seventh stage (nanoparticle- R : gas constant [8.314 J/mol K]
stabilized emulsion/polymer/water flooding) achieved r : droplet radius [µm]
t h e h i g h e s t r e c ove r y, b e c a u s e t h e v i s c o s i t y o f Soi : initial oil saturation [%]
Sof : final oil saturation [%]
nanoparticle-stabilized emulsion is much higher than T : temperature [K]
that of crude oil and solid-free emulsion. In addition, <Greeks>
injection of polymer was injected into the micromodel θow : contact angle [°]
caused oil movement by piston-like displacement and © : viscosity [cP]
decreased viscous fingering effects. ∆P12 : difference in internal pressure between droplets [Psia]
γow : interfacial tension [mN/m]
Micromodel flooding tests demonstrated the success-
ful application of the glass micromodel for studying
enhanced oil recovery techniques. In our experiments, References
emulsion and nanoparticle-stabilized emulsion showed
higher recovery efficiency because of the higher emul- 1) Moeini, F., Hemmati-Sarapardeh, A., Ghazanfari, M.-H.,
Masihi, M., Ayatollahi, S., Fluid Phase Equilib., 375, 191
sion viscosity which caused lower mobility ratio and (2014).
lower viscous fingering effect. Consequently, 2) Hemmati-Sarapardeh, A., Ayatollahi, S., Zolghadr, A.,
nanoparticle-stabilized emulsion flooding provides a Ghazanfari, M.-H., Masihi, M., J. Chem. Eng. Data, 59, 11
viable method to push highly viscous oil from the (2014).
subterranean formation. Moreover, emulsion and 3) Green, D. W., Willhite, G. P., “Enhanced oil recovery,” Society
of Petroleum Engineers Richardson, TX (1998), pp. 124-251.
nanoparticle-stabilized emulsion have lower interfacial 4) Sheng, J., “Modern chemical enhanced oil recovery: theory
tension than water and polymer. and practice,” Gulf Professional Publishing, (2010), pp. 130-
141.
4. Conclusion 5) Maghzi, A., Kharrat, R., Ghazanfari, M., Transp. Porous Med.,
87, (3), 653 (2011).
6) Nilsson, M. A., Kulkarni, R., Gerberich, L., Hammond, R.,
The present study investigated the effect of nano- Singh, R., Baumhoff, E., J. Non-Newtonian Fluid Mech., 202,
particle on the viscosity and stability of emulsions. A 112 (2013).
series of emulsions and nanoparticle-stabilized emul- 7) Willhite, G. P., “Waterflooding,” Society of Petroleum, (1986),
sions were injected into a glass micromodel. Micro- pp. 61-89.
model flooding experiments were performed at a fixed 8) Mai, A., Kantzas, A., J. Can. Petrol. Technol., 49, (3), 44
(2010).
flow rate and at ambient pressure and temperature. 9) Feng, H., Kang, W., Zhang, L., Chen, J., Li, Z., Zhou, Q., Wu,
Viscosity measurements of water-in-oil emulsions H., J. Pet. Sci. Eng., 171, 974 (2018).
indicated that the viscosities increased with the addition 10) McAuliffe, C. D., J. Petrol. Tech., 25, (06), 727 (1973).
of nanoparticles and higher water volume fraction. 11) Fanun, M., “Microemulsions: properties and applications,”
Nanoparticles decreased the IFT between crude oil and CRC Press, (2010), pp. 36-78.
12) Bragg, J. R., Elspass, C. W., Peiffer, D. G., Varadaraj, R., U.S.
water, stabilized the prepared emulsion, and increased Pat. 7186673 (2007).
the emulsion viscosity. The nanoparticles reduced the 13) Kele o lu, S., Pettersen, B. H., Sjöblom, J., J. Pet. Sci. Eng.,
diameter of the emulsion droplets, so that nanoparticle- 100, 14 (2012).
stabilized emulsions flowed more easily through the 14) Son, H., Kim, H., Lee, G., Kim, J., Sung, W., Korean J. Chem.
porous media and increased the capillary numbers. Eng., 31, (2), 338 (2014).
15) Zhang, T., Davidson, D., Bryant, S. L., SPE improved oil
Viscous fingering phenomena occurred during water- recovery symposium, Oklahoma, January 2010, Abstr. No.
flooding, resulting in relatively lower sweep efficiency. SPE 129885.
Emulsion flooding was effective for the recovery of a 16) Tshilumbu, N. N., Kharatyan, E., Masalova, I., J. Dispersion
significant amount of residual oil. Emulsion flooding Sci. Technol., 35, (2), 283 (2014).

J. Jpn. Petrol. Inst., Vol. 62, No. 3, 2019


135

17) Mejia, A. F., Diaz, A., Pullela, S., Chang, Y.-W., Simonetty, M., 19, (3-4), 373 (2001).
Carpenter, C., Soft Matter., 8, (40), 10245 (2012). 32) Yaghi, B., J. Pet. Sci. Eng., 40, (3), 103 (2003).
18) Binks, B. P., Whitby, C. P., Coll. Surf. A, 253, (1), 105 (2005). 33) Simon, S., Theiler, S., Knudsen, A., Sjöblom, J., J. Dispersion
19) Zhang, J., Xu, J.-Y., Gao, M.-C., Wu, Y.-X., J. Dispersion Sci. Sci. Technol., 31, (5), 632 (2010).
Technol., 34, (8), 1148 (2013). 34) Pajouhandeh, A., Kavousi, A., Schaffie, M., Ranjbar, M., Coll.
20) Maia Filho, D. C., Ramalho, J. B., Spinelli, L. S., Lucas, E. F., Surf. A, 520, 597 (2017).
Coll. Surf. A, 396, 208 (2012). 35) Pajouhandeh, A., Kavousi, A., Schaffie, M., Ranjbar, M., S.
21) Andresen, M., Stenius, P., J. Dispersion Sci. Technol., 28, (6), Afr. J. Chem., 69, 113 (2016).
837 (2007). 36) Karambeigi, M., Schaffie, M., Fazaelipoor, M., Pet. Sci.
22) Malkin, A. Y., Masalova, I., Slatter, P., Wilson, K., Rheol. Acta, Technol., 31, (9), 923 (2013).
43, (6), 584 (2007). 37) Youssif, M. I., El-Maghraby, R. M., Elgibaly, A., Egypt. J.
23) Chatenever, A., Calhoun Jr., J. C., J. Petrol. Tech., 4, (06), 149 Petrol., 27, (1), 105 (2018).
(1952). 38) Li, S., Hendraningrat, L., Torsaeter, O., International Petroleum
24) Mattax, C., Kyte, J., Oil Gas J., 2, (2), 177 (2009). Technology Conference, Beijing, March 2013, Abstr. No.
25) Davis Jr., J., Jones, S., J. Petrol. Technol., 20, (12), 415 (1968). IPTC 16707.
26) Abedi, B., Ghazanfari, M. H., Kharrat, R., Energ. Explor. 39) Oliveira, R., Goncalves, M., Offshore Technology Conference,
Exploit., 30, (5), 689 (2012). Houston, May 2005, Abstr. No. OTC 17386.
27) Ashrafizadeh, M., Ramazani, S. A., Sadeghnejad, S., Energ. 40) Hemmati-Sarapardeh, A., Shokrollahi, A., Tatar, A.,
Explor. Exploit., 30, (6), 915 (2012). Gharagheizi, F., Mohammadi, A. H., Naseri, A., Fuel, 116, (1),
28) Moradi, F., Rahmanifard, H., Schaffie, M., Energ. Source Part 39 (2014).
A, 36, (6), 582 (2014). 41) Hajirezaie, S., Pajouhandeh, A., Hemmati-Sarapardeh, A.,
29) Gogarty, W., Littleton, Olson, R. W., U.S. Pat. 3254714 (1966). Pournik, M., Dabir, B., J. Mol. Liq., 229, 89 (2017).
30) Putz, A., Chevalier, J., Stock, G., Philippot, J., J. Petrol. 42) Hemmati-Sarapardeh, A., Aminshahidy, B., Pajouhandeh, A.,
Technol., 33, (04), 710 (1981). Yousefi, S. H., Hosseini-Kaldozakh, S. A., J. Taiwan Inst.
31) Yaghi, B., Benayoune, M., Al-Bemani, A., Pet. Sci. Technol., Chem. Eng., 59, 1 (2016).

J. Jpn. Petrol. Inst., Vol. 62, No. 3, 2019

You might also like