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Egyptian Journal of Petroleum xxx (2017) xxx–xxx

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Egyptian Journal of Petroleum


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Full Length Article

Silica nanofluid flooding for enhanced oil recovery in sandstone rocks


Magda I. Youssif a, Rehab M. El-Maghraby b,⇑, Sayed M. Saleh c, Ahmed Elgibaly d
a
Petroleum Department and Gas Technology, Faculty of Engineering, British University, Egypt
b
Chemical Engineering and Petroleum Refining Department, Faculty of Pet. and Min. Engineering, Suez University, Egypt
c
Department of Science and Mathematics, Faculty of Pet. and Min. Engineering, Suez University, Egypt
d
Petroleum Engineering Department, Faculty of Pet. and Min. Engineering, Suez University, Egypt

a r t i c l e i n f o a b s t r a c t

Article history: Enhanced oil recovery is proposed as a solution for declining oil production. One of the advanced trends
Received 26 September 2016 in the petroleum industry is the application of nanotechnology for enhanced oil recovery. Silica nanopar-
Revised 26 December 2016 ticles (SiNPs) are believed to have the ability to improve oil production, while being environmentally
Accepted 24 January 2017
friendly and of natural composition to sandstone oil reservoirs.
Available online xxxx
In our work, we investigated the effect of silica nanoparticles flooding on the amount of oil recovered.
Experiments were carried using commercial silica of approximately 20 nm in size. We used sandstone
Keywords:
cores in the core flooding experiments. For one of the cores tertiary recovery is applied where brine imbi-
Enhanced oil recovery (EOR)
Porous media
bition was followed by nanofluid imbibition. While in the other cores secondary recovery was applied
Dispersed silica nanoparticle where primary drainage is directly followed by nanofluid imbibition. We investigated the effect of con-
Nanoflooding centration of nanofluid on recovery; in addition, residual oil saturation was obtained to get the displace-
Nanoparticles stability ment efficiency. Silica nanofluid of concentration 0.01 wt%, 0.05 wt%, 0.1 wt% and 0.5 wt% were studied.
Nanofluid The recovery factor improved with increasing the silica nanofluid concentration until optimum concen-
tration was reached. The maximum oil recovery was achieved at optimum silica nanoparticles concentra-
tion of 0.1 wt%. The ultimate recovery of initial oil in place increased by 13.28% when using tertiary
flooding of silica nanofluid compared to the recovery achieved by water flooding alone. Based on our
experimental study, permeability impairment was investigated by studying the silica nanoparticles con-
centration, and the silica nanofluid injection rate. The permeability was measured before and after nano-
fluid injection. This helped us to understand the behavior of the silica nanoparticles in porous media.
Results showed that silica nanofluid flooding is a potential tertiary enhanced oil recovery method after
water flooding has ceased.
Ó 2017 Egyptian Petroleum Research Institute. Production and hosting by Elsevier B.V. This is an open
access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

1. Introduction and structural properties of the nanomaterial differs totally from


those displayed by either their atoms or the bulk materials [3].
Due to the declining oil production in many oil reservoirs, For enhanced oil recovery purpose, the smaller the nanoparticle
advanced techniques are necessary to continue oil production size, the larger the surface area, and the larger the contact surface
and to recover more oil in place [1]. Among those techniques are between the nanoparticles and the oil phase. This allows better
the enhanced oil recovery techniques. The use of nanotechnology interaction between the nanoparticles and the oil phase for further
for enhanced oil recovery is considered to be a new emerging recovery [4]. The most commonly used nanoparticles in enhanced
trend. This nanotechnology application began at the end of oil recovery are silica nanoparticle (SiNPs). About 99.8% of silica
1980’s and has been developed to synthesize new nanomaterials nanoparticle are silicone dioxide, which is the main component
by rearranging atoms and molecules [2]. Based on the small size of sandstone. Silica nanoparticles are an environmentally friendly
of the nanoparticles (1–100 nm), the optical, thermal, chemical, material compared to other nanomaterials. In addition, silica
nanoparticles are cheap and their chemical behavior could be
easily controlled by surface modification.
Peer review under responsibility of Egyptian Petroleum Research Institute. There are possible displacement mechanisms, by which silica
⇑ Corresponding author. nanoparticle could enhance oil production, are believed to occur.
E-mail addresses: magda.ibrahim@bue.edu.eg (M.I. Youssif), rehab.elmaghraby@ The first mechanism is the disjoining pressure mechanism. This
suezuniv.edu.eg (R.M. El-Maghraby), sayed.saleh@suezuniv.edu.eg (S.M. Saleh),
mechanism occurs when silica nanoparticle are present in the dis-
Elgibalya@yahoo.com (A. Elgibaly).

http://dx.doi.org/10.1016/j.ejpe.2017.01.006
1110-0621/Ó 2017 Egyptian Petroleum Research Institute. Production and hosting by Elsevier B.V.
This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

Please cite this article in press as: M.I. Youssif et al., Silica nanofluid flooding for enhanced oil recovery in sandstone rocks, Egypt. J. Petrol. (2017), http://dx.
doi.org/10.1016/j.ejpe.2017.01.006
2 M.I. Youssif et al. / Egyptian Journal of Petroleum xxx (2017) xxx–xxx

persing medium, so these particles tend to rearrange themselves in Dioxide (TiO2) 60.03%, Hydrogen Chloride (HCl) 60.028% and other
a wedge-shaped film in contact with the discontinuous oil phase traces elements.
[5,6]. The wedge film acts to detach the oil phase from the rock sur- Hydrophilic silica nanoparticles were suspended in 3 wt% brine;
face, hence recovering more oil as illustrated in Fig. 1. The disjoin- this solution will be referred as silica nanofluid. The Nanofluid was
ing pressure represents the pressure difference between the prepared with different concentrations, 0.01 wt%, 0.05 wt%, 0.1 wt
pressure in the wedge film region and that in the bulk liquid [7]. %, 0.2 wt% and 0.5 wt%. Each solution was mixed by using magnetic
This pressure is driven by Brownian motion and the electrostatic stirrer for several minutes. To avoid precipitation of nanoparticles
repulsion between molecules. from solution, ultrasonic probe (400 W and 0.5 Hz) is used for 1 h
The second mechanism is the Log-Jamming mechanism. Due to to assurance the homogeneity and stability of prepared solutions.
the smaller size of pore throats and the constant differential pres- The properties of the used nanofluid at different silica nanoparti-
sure in the pores, the velocity of the silica nanofluid will increase at cles concentrations are listed in Table 2.
the pore throat compared to the pore body. This may cause the
water molecules to move faster than the silica nanoparticles, caus- 2.2. Methodology
ing the nanoparticles to accumulate and eventually block the pore
entrance. This may force the water flow to change pass to other The equipment used for cores flooding was manufactured by
non-invaded pores, possibly oil filled, resulting in more oil recov- Vinci Company, in France. The experimental set-up is shown in
ery. The third mechanism is the wettability alteration mechanism. Fig. 2. Two flooding scenarios were studied; one with silica nano-
Silica nanoparticles have the ability to change rock wettability and fluid as a secondary recovery technique, and the other where silica
to reduce the interfacial tension and the contact angle between nanofluid are used as a tertiary recovery technique.
two immiscible fluids [1,8–10]. In the first scenario, silica nanofluid were used as a tertiary
Oil recovery by nanofluid flooding is affected by various param- recovery technique. Core# 1 was first cleaned and dried then
eters such as nanofluid concentration, particle size, injection rate, placed in glass desiccator to be fully saturated with brine of 3 wt
and slug size. Nanofluid concentration is considered one of the % NaCl concentration. The weight of the core was recorded many
major parameters to enhance oil recovery. The goal of this study times until the weight remained constant. The core was placed in
is to investigate the effect of silica nanofluids as an enhanced oil the core holder and black oil injection took place. The injection
recovery agent in Sandstone rocks. flow rate was increased until irreducible water saturation was
reached. At this point the core was saturated with oil. Then
imbibition process was initiated by using brine to displace oil at
2. Materials and methodology
injection rate of 0.5 ml/min, and then continued until no more oil
produced. Pore volume of the injected brine was 1.77 PV. At this
2.1. Materials
stage, residual oil saturation (Sor1) was determined, and recovery
factor was calculated. The next step was to continue injection
Three Sandstone cores of different permeability ranges were
by nanofluid of different concentration at injection rate of
used. The properties of the cores are listed in Table 1. Black oil of
0.5 ml/min. At this stage, residual oil saturation (Sor2) was deter-
32.5 API and 4.6 cp obtained from the North Sea was used in the
mined again, and recovery factor was calculated to determine
flooding experiments. The synthetic brine used is of concentration
how much oil would be produced at this concentration.
of 3.0 wt% NaCl (GPR grade, purity 99.5%, from Alpha Chemicals
The displacement efficiency was calculated from the following
Company).
equation:
Commercial hydrophilic mono dispersed silica (SiO2) nanoparti-
 
cles of 370 m2/g specific area were used in the experiments. The Sor2
ED ¼ 1   100 ð1Þ
average particle size was 22 nm. They consist of basically more Sor1
than 99.8% of silicon dioxide (SiO2) (Al2O3) 60.06%, Titanium

Fig. 1. Illustration of nanoparticle schematic and structural disjoining pressure gradient mechanism among solid, oil and nanofluids as aqueous phase.

Please cite this article in press as: M.I. Youssif et al., Silica nanofluid flooding for enhanced oil recovery in sandstone rocks, Egypt. J. Petrol. (2017), http://dx.
doi.org/10.1016/j.ejpe.2017.01.006
M.I. Youssif et al. / Egyptian Journal of Petroleum xxx (2017) xxx–xxx 3

Table 1
The properties of the sandstone cores used in our experiments.

Core No. Length Diameter Pore volume Porositya Permeabilityb Swi


(cm) (cm) (cc) % md %
Core# 1 4.2 3.8 8.9 19.4 587 10.0
Core# 2 4.1 3.8 9.9 21.7 285 23.7
Core# 3 4.3 3.8 9.5 19.8 325 16.2
a
Porosity is measured by Helium Porosimeter.
b
Permeability is measured by Klinkenberg method.

Table 2 the permeability impairment [12]. The permeability was measured


Silica nanofluid properties. before and after nanofluid injection on Core# 1, Core# 2, and Core#
Fluid Density, gm/cc Viscosity, cp 3 to make sure that permeability impairment or other reduction in
Nanofluid 0.01 wt% 1.019 1.009
reservoir properties didn’t exceed a desired value.
Nanofluid 0.05 wt% 1.019 1.067
Nanofluid 0.1 wt% 1.020 1.160
Nanofluid 0.5 wt% 1.022 1.347 3. Results & discussion

Tertiary recovery is performed on Core# 1, after imbibition by


where, ED is displacement efficiency, Sor1 is residual oil saturation water flooding; Core# 1 was flooded by silica nanofluid of different
after brine floods, and Sor2 is residual oil saturation after nanofluid concentration. Fig. 3 showed the relation between PV injected and
floods. recovery factor at each concentration for Core# 1. The residual sat-
In the second scenario, Core # 2 and Core# 3 were tested using uration after water flooding and silica nanofluid flooding for core#
silica nanofluid as secondary recovery method. The previous flood- 1 and core# 2 are listed in Table 3. It was observed that the injec-
ing steps mentioned in scenario 1 were repeated. The only differ- tion of silica nanofluid in the core enhances oil production, espe-
ence was that the imbibition step using brine was not followed cially as the silica concentration increases. The higher the silica
immediately by silica nanofluid imbibition. Instead after the imbi- concentration, the higher the amount of recovered oil up to an
bition of the core with brine the core was cleaned, then dried and optimum silica nanofluid concentration after which the oil recov-
saturated with brine. The drainage process was initiated by oil ery decrease. It is believed that permeability impairment was the
injection in the core till irreducible water saturation is reached, cause of the reduction in oil recovery at high concentration
after which the silica nanofluid imbibition stared immediately till because of the locking of the tiny pores of the core plug. The use
we reach residual oil saturation. Different silica nanofluid concen- of silica nanoparticles following brine flooding increased the oil
tration was investigated. recovery factor from 53.1% in the case of water flooding alone to
Injecting Silica nanoparticles through the pores of the cores may 66.40% following silica nanofluid injection at 0.1 wt% silica concen-
lead to particle retention in some cases [11]. Consequently many tration as a tertiary recovery.
parameters should be taken into consideration to eliminate perme- Secondary recovery is performed on Core# 2, where the primary
ability impairment to minimum level. Concentration of nanoparti- drainage stage is followed by direct silica nanofluid imbibition. Dif-
cle suspension, well-dispersion solution, injection rate, and pore ferent silica nanoparticles concentrations were used to reach an
volume injected are the most important parameter affecting on optimum concentration that will maximize the oil recovery factor.

Fig. 2. Experimental set up schematic: (1) Graduated tube. (2) Prep Pump. (3) Injection pipe. (4) Core holder. (5) Core plug. (6) Sleeve pressure. (7) Fluid accumulator. (8)
Carry over fluid accumulator. (9) Hydraulic pump.

Please cite this article in press as: M.I. Youssif et al., Silica nanofluid flooding for enhanced oil recovery in sandstone rocks, Egypt. J. Petrol. (2017), http://dx.
doi.org/10.1016/j.ejpe.2017.01.006
4 M.I. Youssif et al. / Egyptian Journal of Petroleum xxx (2017) xxx–xxx

70

60

Oil recovery of IOIP, %


50
WF

40 NF, conc 0.01wt.%


NF, Conc 0.05%
30
NF, conc. 0.1wt.%
20 NF,conc. 0.5 wt.%

10

0
0 1 2 3 4 5 6
PV injected

Fig. 3. Recovery factor (RF) vs. pore volume (PV) injected for Core # 1

Table 3
Residual oil saturation (Sor) obtained after water flooding and Silica nanofluid flooding.

Oil saturation [ So], fraction


Core Before water After water After 0.01 wt% After 0.05 wt% After 0.1 wt% After 0.2 wt% After 0.5 wt%
No. flooding flooding nanoflooding nanoflooding nanoflooding nanoflooding nanoflooding
Core 1 0.9 0.422 0.408 0.34 0.302 – 0.416
Core 2 0.763 0.447 – 0.383 0.351 0.397 0.465

As shown in Fig. 4, the optimum silica concentration was 0.1 wt%. tonation of these silanol groups. The resultant net charge of silica
At this concentration an oil recovery factor of 54% was achieved nanoparticles surface controls to which extent the repulsion forces
compared to an oil recovery factor of 41.3% in the case of water keep particles dispersed in solution. The drop in the oil recovery, in
imbibition alone. case of increasing the concentration of silica nanoparticles in pres-
Introducing silica nanoparticles to the oil/water system was ence of constant electrolyte concentration, may be due to the
observed to lower the interfacial tension (IFT), then the potential increment of the deprotonation process of silanol groups at the
to produce more trapped oil [13,14]. This may be due to the hydro- surface of nanoparticles which accelerates the coagulation process
philic part of the silica nanoparticles present in the aqueous phase forming a cumulative particles that block the pores hindering oil
and the hydrophobic part exists in the oil phase, so the adhesive production.
forces between the two phases increases and the IFT decreases. Comparing flooding in Core# 1 and flooding in Core# 2 we can
It was observed that within the range of silica nanoparticles see that there is no difference in the recovery when using silica
concentration of 0.2 and 0.5 wt% there is a drop in the oil recovery nanofluid in a secondary recovery technique or in a tertiary recov-
when compared to the trend of other silica concentrations. As silica ery technique, as at the end we get nearly the same results. As we
surface is completely hydroxylated and each Si atom on the surface can see from Fig. 3 an increase of 13.28% in the oil recovery was
is surrounded by OH groups [15], the surface charge of the silica achieved when the silica tertiary recovery technique was followed
nanoparticles were determined in terms of protonation and depro- by water secondary recovery technique in Core #1. We can also see

60

50 WF

40 NF, Conc
0.05wt.%
NF, conc 0.1wt%
RF , %

30

NF, conc. 0.2wt%


20
NF, conc. 0.5wt.%

10

0
0 1 2 3 4 5 6
PV injected

Fig. 4. Recovery factor (RF) vs. pore volume (PV) injected for Core # 2.

Please cite this article in press as: M.I. Youssif et al., Silica nanofluid flooding for enhanced oil recovery in sandstone rocks, Egypt. J. Petrol. (2017), http://dx.
doi.org/10.1016/j.ejpe.2017.01.006
M.I. Youssif et al. / Egyptian Journal of Petroleum xxx (2017) xxx–xxx 5

from Fig. 4, an increase of 12.7% in oil recovery factor was achieved amount of oil that could be recovered. However, as the concentra-
when using silica nanofluid flooding as a secondary recovery tech- tion of nanoparticle in fluid increase the porosity and permeability
nique compared to using water flooding as a secondary recovery is affected causing permeability impairment [12]. Hence, the
technique in Core# 2. This result will favour using water flooding important to work at 0.1 wt% silica nanofluid concentration, to
as a secondary recovery technique due to its low price and feasibil- achieve the maximum oil recovery with minimum permeability
ity at the start of the recovery, then silica nanofluid flooding can be impairment.
used as a tertiary technique to utilize the benefit of silica nanopar-
ticles in enhancing the oil production. 3.1. Permeability impairment
In addition, recovery achieved by nanofluid of concentration
0.5 wt% is less than that achieved by water flooding. This is mainly Permeability was calculated using Darcy equation. The effect of
due to the accumulation of the silica nanoparticles through the nanoparticles concentration and injection rate on the permeability
pores and pores throats, hence blocking the pores. Consequently, impairment was studied.
this concentration could not be applicable as it could damage the
rock morphology. 3.1.1. Effect of concentration
Core flooding is carried on Core# 3 to investigate the effect of Based on the results shown in Table 4, as the concentration of
silica nanofluid on water breakthrough. As shown in Fig. 5, it was silica nanofluid increases the absolute permeability decreases, at
observed that silica nanofluid has an effect on delaying water constant nanofluid injection rate of 0.5 ml/min. Maximum perme-
breakthrough; hence volumetric sweep efficiency increase and ability reduction of 60% due to nanofluid injection was observed at
more oil could be produced as confirmed also by Li and Torsaeter 0.5 wt% silica nanofluid concentrations. This result justifies that at
[10]. The experiments were done at concentration of 0.1 wt% and 0.5 wt% nanofluid concentration the oil recovery by silica nanofluid
at constant injection rate of 0.5 ml/min. was the lowest of all concentration due to pore blockage.
In general, when the concentration of the silica nanofluid
increases within specific range, the random movement of particles 3.1.2. Effect of injection rate
increases [7], thereby repulsive forces between molecules increase Nanoparticles retention is affected by the silica nanofluid injec-
and the rock wettability is strongly altered. This will increase the tion rate. Due to the high velocity and the difference in density

100

80
WF
W/C , %

60
NF, conc.
0.1wt.%
40

20

0
0 1 2 3 4 5 6
PV injected

Fig. 5. Water cut vs. pore volume (PV) injected for Core# 3.

Table 4
Effect of silica nanoparticle concentration on permeability impairment at 0.5 ml/min injection rate.

Core No. k absolute before nanofluid injection Silica nanofluid concentration. k absolute after nanofluid injection k reduction
md [%] md [%]
Core# 2 285 0.05 231 19
Core# 3 325 0.1 195 40
Core# 1 587 0.5 233 60

Table 5
Effect of silica nanoparticle injection rate on permeability impairment at 0.05 wt% silica concentration.

Core No. k absolute before nanofluid injection Silica nanofluid injection rate k absolute after nanofluid injection k reduction
md [cc/min] md [%]
Core# 2 285 0.2 203 29
Core# 3 325 0.5 149 54
Core# 1 587 0.8 154 74

Please cite this article in press as: M.I. Youssif et al., Silica nanofluid flooding for enhanced oil recovery in sandstone rocks, Egypt. J. Petrol. (2017), http://dx.
doi.org/10.1016/j.ejpe.2017.01.006
6 M.I. Youssif et al. / Egyptian Journal of Petroleum xxx (2017) xxx–xxx

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Please cite this article in press as: M.I. Youssif et al., Silica nanofluid flooding for enhanced oil recovery in sandstone rocks, Egypt. J. Petrol. (2017), http://dx.
doi.org/10.1016/j.ejpe.2017.01.006

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