Fuel 267 (2020) 117262

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Review article

Application of bare nanoparticle-based nanofluids in enhanced oil recovery T

a,c,⁎ b,⁎
Mohamad Sahban Alnarabiji , Maen M. Husein
a
Department of Chemical Engineering, Universiti Teknologi PETRONAS, Bandar Seri Iskandar, 31750 Tronoh, Perak, Malaysia
b
Department of Chemical & Petroleum Engineering, University of Calgary, Calgary, AB T2N 1N4, Canada
c
Department of Petroleum Engineering, Universiti Teknologi PETRONAS, Bandar Seri Iskandar, 31750 Tronoh Perak, Malaysia

A R T I C LE I N FO A B S T R A C T

Keywords: Nanofluids offer many advantages over surfactant and polymer solutions during enhanced oil recovery (EOR).
Nanofluid This review discusses the current state and future prospects of nanofluids consisting of bare nanoparticles (NPs)
Interfacial tension in aqueous media and their application in EOR. The following topics are addressed: advantages and challenges of
Reservoir bare and functionalized nanofluid injection, observations on NP mobility within reservoirs as well as mechan-
Nanoparticle
isms pertaining to nanofluid EOR. The role of the NP chemical nature, size, size distribution, surface charge,
Mobility
isoelectric point and concentration is thoroughly reviewed. The impact of factors such as high temperature, pH,
EOR
salinity and the nature of reservoir rock surface are highlighted in order to provide a better understanding and
ability to predict EOR rate of nanofluid injection. Potential synergy among the different NP characteristics is
gaged through experimental results from multiple research clusters. The proposed mechanisms; namely reduc-
tion of interfacial tension, increment in viscosity, in situ formation of Pickering emulsion and/or alteration of the
disjoining pressure and wettability are critically discussed. Future work in this field should address the following
gaps; (1) precise determination of the isoelectric point of the NPs under reservoir conditions; (2) workable
measurement to faithfully capture particle size distribution; (3) a mean to correlate aging time of the NPs in the
base fluid under reservoir environment; and (4) exploring the fine balance between surface charge needed to
stabilize the particles while maintain their effectiveness as interfacial tension modifiers.

1. Introduction electromagnetic and electrical heating can be classified under thermal

Fossil fuels have been the main source of energy over the past three
centuries. Fossil fuels offer many advantages over other alternative
energy sources such as high energy density, suitability as transportation
fuel as well as established platform for production, transportation and
commodity exchange [1–3]. In 2008, the global economic crises arose
due to a persistent decline in oil extraction from the existing fields
coupled with a decreased interest in the discovery of new oil reserves
[4,5].
Tertiary recovery, commonly known as enhanced oil recovery
(EOR), refers to the recovery of trapped oil in the reservoir following
primary and secondary recovery processes. To date, on average, only
30–40% of the original oil in place (OOIP) is recovered successfully by
applying different methods such as thermal, gas injection, and chemical
flooding. Almost 60–70% of the OOIP is still trapped within reservoir
pores and channels. Increasing the production by just 5% has been
challenging for conventional EOR processes [6]. Conventional tertiary
recovery could be divided into three main groups: miscible flooding,
chemical flooding, and thermal methods. Steam injection,
methods [7]. In these methods high temperature is used to reduce the
viscosity of the viscous oil. However, the high energy penalty generally
makes these methods a tough choice [7]. On the other hand, the use of
miscible flooding, where various types of solvents mix up with the
trapped oil to enhance its recovery, is growing. Gas injection, which
depending on the pressure may be classified as miscible flooding, in-
volves injecting a gas such as high-pressure carbon dioxide, nitrogen,
flue gas, liquefied petroleum gas, methane and methane mixed with
light hydrocarbon. However, gas displacement methods are limited to
deep deposits. Hence, they require sufficiently deep reservoirs, nearly
5000 ft for the highest pressure and 2000 ft for the lowest pressure [8].
The major obstacle, nevertheless, is the drastic decline in the dis-
placement efficiency encountered for high oil viscosity and density due
to fingering of the gas through the oil. This renders gas injection only
economical for the lighter end of the heavy oil [7]. Lastly, during
chemical flooding, surfactants, alkalis and/or polymers are mixed with
water in different ratio and injected into the target reservoir in order to
improve the sweep efficiency and reduce the interfacial tension [9,10].
High recovery can be achieved, up to 40%, using this technique.

⁎
Corresponding authors.
E-mail addresses: mohamad.alnarabiji@utp.edu.my, mohamad.alnarabiji@gmail.com (M.S. Alnarabiji), mhusein@ucalgary.ca (M.M. Husein).

https://doi.org/10.1016/j.fuel.2020.117262
Received 10 November 2019; Received in revised form 5 January 2020; Accepted 30 January 2020
0016-2361/ Crown Copyright © 2020 Published by Elsevier Ltd. All rights reserved.
M.S. Alnarabiji and M.M. Husein
Nomenclature
List of abbreviations and symbols
D Brownian diffusion coefficient
EOR Enhanced oil recovery
ER Electrorheological
HLPN Hydrophobic and lipophilic polysilicon
IEP Isoelectric point
IFT Interfacial tension
k Boltzmann constant (1.38064852 × 10−23
m2.kg.s−2.K−1)
However, chemical flooding suffers the high cost of makeup chemicals
as a result of adsorption onto reservoir rocks such as carbonates and
clay rocks [7]. Moreover, chemical flooding is also limited by the sus-
ceptibility of the different chemicals to degradation at the harsh re-
servoir conditions [11,12]. Comprehensive understanding of the bio-
degradation route of some types of surfactants/polymers is crucial as
their toxicity might increase at certain reservoir conditions. For in-
stance, surfactants from alkyl benzene sulfonates (linear) are aquatic
toxins, and water hardness and salinity may increase their toxicity [13].
All of the above limitations constituted a need for a new, more robust
recovery methods.
Nanoparticles (NPs) have been implemented in EOR in the form of
foams, hydrosols and/or organosols in order to capitalize on NP at-
tractive features; including their high surface area and mobility as well
as relative ease of preparation [14,15]. In order to improve NP dis-
persion and characteristics, especially under the harsh reservoir en-
vironment, it was mixed with different types of surfactants and poly-
mers [16–20]. For instance, phosphonates, as a class of surfactants,
have been commonly used to coat NPs [21,22]. Nevertheless, the field
application of phosphonates, and many other polymers, was hindered
because of their failure to meet minimum biodegradation requirements
[23,24]. More generally, reducing the number of additives reduces the
cost and the complexity of an operation.
In this review, the challenges facing the application of nanofluids
consisting of bare NPs, i.e. without surfactant and/or polymer, in EOR
are summarized and critically analyzed. Pertinent parameters of NP
type, size, size distribution, surface charge, isoelectric point (IEP),
concentration and physicochemical properties are extensively re-
viewed. In addition to the reduction in the interfacial tension and in-
crement in viscosity of the injected fluid, other recovery mechanisms
such as alteration of the disjoining pressure and wettability as well as in
situ formation of Pickering emulsion are discussed in detail. This review
also attempts to carve pathways for future research on the application
of nanofluids in EOR. These pathways are based on comprehensive
analysis of the characteristics of the NPs and their impact on the re-
sultant nanofluid.
2. Why nanofluid?
The use of nanofluids in oil and gas industry has steadily grown over
the past decade [25–30]. Li et al. [31] published a detailed review of
nanofluid preparation. Nanofluids display more attractive features over
traditional sols and surfactant colloidal systems. Suspensions of nano-
scaled materials display high stability against sedimentation, relative to
microscale suspensions, owing to high extent surface forces which
preserves the particles against aggregation, allowing entropic forces to
easily counter balance the force of gravity [32]. Long term stability of
the sol can be achieved through using an appropriate stabilizer or by
phase transfer of the NPs from an aqueous carrier into an organic
medium [32]. Moreover, the main characteristics of nanofluids; in-
cluding optical, stress-strain, thermal, rheological, magnetic and
2
Fuel 267 (2020) 117262
LDH Layered double hydroxide
LHPN Lipophobic and hydrophilic
ME Magnetorheological
MWCNT Multi walled carbon nanotubes
NCs Nanocrystals
NPs Nanoparticles
T Absolute temperature (K)
Greek letters
µ Viscosity of the fluid (Pa.s)
electrical properties can be engineered by modifying the morphology
and/or the size of the NPs during the synthesis process [33,34]. As such,
nanofluids may be engineered to maximize the production of trapped
oil from reservoirs through controlling their surface and rheological
properties [35]. Several studies were conducted to achieve a better
understanding of the behavior of the NPs at the oil-water interface. For
example, Line et al. [36] studied the dispersion of NPs, specifically
CdSe, in toluene and water phases. The experimental results showed
that NPs effectively disperse at the interface. The effect of Bi2Ti3 par-
ticle size and concentration on the interfacial tension showed that
smaller particles are better able to reduce the interfacial tension, and
the interfacial tension decreased with increased NP concentration [37].
Reincke et al. [38] investigated the effect of the surface charge of Au
NPs on the population of the particles at the oil-water interface. They
observed that increasing the surface charge over certain value reduces
the number of particles at the interface. Moreover, the role of the na-
nofluids in emulsion formation, and stability is detailed in Table S1 of
the supplementary material.
Other studies explored the impact of NP dispersions on the viscosity
of the base fluid [39]. It was found that the viscosity of the base fluid
increased upon effective dispersion of the NPs. NPs may change the
rheological properties of an emulsion from a Newtonian fluid, where
the viscosity of the fluid depends on the composition, pressure and
temperature, to a non-Newtonian fluid, where the viscosity of the fluid
can also be affected by the flow conditions [40,41]. The apparent
viscosity of non-Newtonian fluids may be higher or lower than the
viscosities of its constituent fluids [42]. Therefore, in situ formation of a
non-Newtonian fluid with higher viscosity upon emulsification of
trapped oil may result in a better sweep efficiency relative to the in-
jected fluid [43]. The resultant fluid may better be able to overcome the
capillary forces and displace the oil in the form of “piston-like” me-
chanism instead of passing through the oil forming “finger-like” region.
2.1. Advantages of NP application in EOR
In the reservoir environment, NPs have many advantages over
larger size colloid particles. When NPs and larger particles are injected
into a porous medium, they both may adsorb onto pore throats.
However, the larger particles are neither able to desorb back nor mi-
grate for long distance within the reservoir environment. The size of the
larger particles is comparable to the pore throat and size exclusion
prevents them from migrating further into the porous medium. NPs, on
the other hand, migrate and pass through most of the reservoir pore
throats by means of bulk flow and Brownian motion [44]. Depending
on the forces of interaction with the pore throat, Brownian motion may
detach the particles after adsorbing onto the pore wall. Brownian dif-
fusion is related to the radius of the particle, Dp , through Stokes-Ein-
stein equation [45].
D = kT /6πμDp (1)
where D is Brownian diffusion coefficient, k is the Boltzmann constant
M.S. Alnarabiji and M.M. Husein Fuel 267 (2020) 117262

(1.38064852 × 10−23 m2.kg.s−2.K−1), T is the absolute temperature
(K), and µ is the viscosity of the fluid (Pa.s). Stokes-Einstein equation is
derived through a balance between diffusion/entropic force and the
viscous force within the Stokes regime. Simulation results showed that
the flow is very slow near a solid wall [46]. Smaller particles have
larger diffusion coefficients and higher mobility. Hence, the residence
time of smaller particles at or near the pore wall is reduced, and their
chances of being adsorbed to the wall are minimized. Moreover, NPs
are better able to stabilize and form “Pickering emulsions” than larger
particles. Lastly, larger colloidal particles tend to plug pore throats
which may damage the reservoir [46].
Different studies showed that different types of bare NPs increase oil
recovery, as summarized in Table 1. The proposed recovery mechan-
isms are included in Table 2. Table 1 suggests that bare SiO2 NPs, with
concentration ranging between 0.05 and 1.00 wt%, have been used in
most of the previous studies and achieved, in general, the highest oil
recovery among the different NPs. Besides the high surface area and
flexibility toward surface modification, SiO2 is native to most reservoirs
[47]. Accordingly, potential environmental contamination, at least due
to the chemical nature of the NPs, may be minimized when bare SiO2 is
used. For instance, Metin et al. [48] reported highly stable bare SiO2
NPs with zeta potential values approaching −45 mV in pH range 6–10.
However, the presence of electrolytes can reduce or weaken the net
repulsion forces between NPs and thus cause the agglomeration and
precipitation of SiO2 particles [49]. On the other hand, SiO2 NPs display
mainly spherical morphology which enables them to pass smoothly
through the pores and channels of the reservoir. In addition, SiO2 NP
size can be controlled based on the synthesis conditions. Of course, the
size of SiO2 NPs must be maintained smaller than the pore size in order
to avoid formation damage [46]. Therefore, SiO2 NPs are attractive
platform for EOR. Lastly, the several possible surface modifications of
the SiO2 NPs allow precise control over the surface chemistry to mod-
ulate NP dispersion [50].
medium, four events may occur based on the particle affinity to the
surface, size and size distribution: adsorption, desorption, transport,
and blockage. Despite their ability to better maneuver in porous media,
relative to microparticles, pore throat blockage is sill one of main
challenges that takes place upon injecting the nanofluid into the porous
medium [68]. An investigation on the effect of particle size distribution
on NP mobility using Sn-Bi particles of < 600 nm injected into Berea
sand stone (porosity = 58%, permeability = 18.1 Darcy and pore vo-
lume = 2.6 cm3) revealed that particles with sizes < 200 nm were able
to pass through the core sample [20]. Few studies, on the other hand,
were performed to explore the impact of particle size on interfacial
tension and emulsion droplet size. Results showed that a decrease in the
interfacial tension and droplet size was attained via decreasing particle
size [37,69,70]. The effect of two different sizes of CdSe; namely 2.8 nm
and 4.6 nm, was investigated on the behavior of the NPs at toluene-
water interface [36]. Results showed that larger size NPs displace
smaller size particles from the toluene-water interface. Therefore, NPs
with narrow size distribution may behave differently than NPs with
wide size distribution on an oil-water interface.
One of the major challenges of NP application in EOR is the eco-
nomical aspect. The cost of NPs hinders the widespread application of
nanofluids in EOR. Husein and coworkers have addressed the cost of
NPs as well as their stability within the nanofluid using an in situ ap-
proach for synthesizing the NPs from inexpensive water-soluble pre-
cursors [71]. Their results also showed promise for applications other
than EOR [72–74].
2.3. The impact of reservoir environment on NPs
Reservoir environment; including salinity, temperature, pH and
reservoir rock chemical and physical nature (e.g. surface charge), has a
major impact on the fate of NPs in a reservoir. The effect of the re-
servoir conditions is detailed below.

2.2. Challenges of NP application in EOR
Most reservoirs are composed of silicate clays, aluminum and ferum
oxides, mineral precipitates, microorganisms, and humic materials
[47]. There are six major forces that govern the performance of the NPs
in the reservoir environment; namely intermolecular forces, disjoining
pressure, surface tension, capillary force, viscous force, gravity force
[66]. The surface film behavior, water distribution, roughness, miner-
alogy, and pore shape of the rock affect NP mobility and adsorption
and, consequently, dominate oil recovery [66,67].
When a dispersion of solid particles is injected into a porous
2.3.1. Impact of the formation fluid salinity
The stability of bare NP dispersions in aqueous solutions depends
strongly on the electrostatic repulsion between same charged surfaces.
High ionic strength in the medium, due to the presence of salts, com-
presses and shrinks the size of the electrostatic double layer leading to
severe reduction in the electrical repulsion between the NPs.
Abundance of ions in the solution may also lead to surface neutraliza-
tion of the charged NPs. Both effects enable the attractive van der Waals
forces to dominate at longer distances [75]. Van der Waals forces are
relatively short range, weak attraction forces between electrically
neutral molecules that collide with or pass so close to each other. These

Table 1
Types of bare NPs used for EOR and the corresponding recovery efficiency.
Reference Nanomaterial Concentration (wt%) Other components Oil recovery %

Alnarabiji et al. [51] MWCNT 0.05 – 31.8

Alnarabiji et al. [30] ZnO 0.10 – 8
Haroun et al. [52] CuO 5.0 electrokinetics (2 V/cm) 81.83
NiO 62.77
Fe2O3 80.49
Hendraningrat et al. [53] SiO2 0.05 – 63.15
Ehtesabi et al. [54] TiO2 0.01 – 80
Onyekonwu and Ogolo [55] Neutrally wet polysilicon nanoparticles ≥ 0.3 – 50–70
hydrophobic wet hydrophobic wet ≥0.3 – 50–81
Kazemzadeh et al. [56] SiO2 0.2 – 22.6
NiO 0.2 – 14.6
Fe2O3 0.2 – 8.1
Hendraningrat and Torsæter [57] SiO2 0.05 – 72.22
Maghzi et al. [58] SiO2 3.0 – 26
Lu et al. [59] SiO2 10 ppm brine 19.5
Yoon et al. [60] SiO2 (12 nm) 1.0 Deionized water 61.4
SiO2 (22 nm) 1.0 63.0
Molnes et al. [61] cellulose nanocrystals 0.5–2.0 1000 ppm NaCl brines –

3
M.S. Alnarabiji and M.M. Husein Fuel 267 (2020) 117262

forces are electrostatic in nature and are displayed as attraction be-

LHPN is not a good agent for EOR in a water wet rock. Therefore, it is recommended to be

For sandstone and dolomite packing, NPs easily pass through without changing the core
cosurfactant, reduces IFT between oil and water and improves oil recovery efficiency.
tween electron-rich regions of one molecule and electron-poor regions

Increasing oil recovery due to wettability alteration caused by structural disjoining

The complimentary effects of NWPN and HLPN with Ethanol which acts as a good
of another [76]. It is important to highlight that the extent of attraction

HLP able to reduce interfacial tension between oil and water and alters the rock
is much weaker than a chemical bond. However, given the close
proximity NPs can get into at the reservoir conditions, van der Waals
forces become important [35]. Accordingly, in a reservoir with high

Hence NWPN and HLPN are good for EOR in water wet formation.
salinity, it is expected that the aggregation and retention of NPs will be
high [14,75,77–81]. In line with this, experimental studies confirmed
that the recovery efficiency is reduced by 10% when nanofluids were

wettability from strongly water wet rock to less water wet.

Higher concentration of NPs in the fluid gives lower IFT.

pumped into a high salinity medium compared with a low salinity one
[79]. Experimental results revealed that when the pre- and post-brine
fluids have lower salinity, the recovery efficiency using nanofluids was
For limestone packing, small adsorption occurs.

significantly higher [14]. When nanofluid injection is used as a tertiary

recovery method following brine injection, mixing takes place due to
the heterogeneity of the pores and the channels which promotes higher
NP agglomeration, adsorption and/or deposition into the porous
medium. Nevertheless, recent work showed that nanocellulose is able to
remain stable in 1 wt% NaCl brine by virtue of its negative surface
used in oil wet formation.

charge [82]. Na-NMR confirmed that Na+ has higher affinity to adsorb
to water molecules than the cellulose functional groups [83,84], since
Na+ is highly hydrophilic. Therefore, Na+ is less likely to neutralize the
permeability.
Major results

nanocellulose surface charge. Divalent and polyvalent cations of the

brine, e.g. Ca2+, on the other hand, selectively attach at the negatively
pressure

charged functional groups [85], which may lead to less stability of the
nanocellulose through surface neutralization.
The effect of salinity on NP stability can also relate to the wettability
Alter rock wettability from hydrophobic to

of the NP surface. At constant NP concentration, salinity had insignif-

between NPs and core sample packing
Electrostatic adsorption and repulsion

icant effect on the water volume fraction of an emulsion formed with

hydrophobic NPs, whereas for hydrophilic NPs the impact was sig-
nificant [86]. The proposed reasoning is that hydrophobic NPs partition
Interfacial tension reduction

Interfacial tension reduction

Interfacial tension reduction

more into the oil phase and, hence are shielded from the high ionic
strength of the aqueous phase, as schematically presented in Fig. 1.
Wettability alteration
Disjoining Pressure

Hydrophilic NPs with abundant surface charges may partition less at

the interface and, hence, are subjected to the destabilizing effect of the
hydrophilic
Mechanism

ionic strength of the aqueous phase.

2.3.2. Impact of the formation pH

The pH of the reservoir is not neutral and differs from one reservoir
ethanol and deionized water

to another [87,88]. On the other hand, the point of zero charge of the
Poly-ethylene glycol 8000

NPs depends on their chemical structure and/or the chemical nature of

Brine with 2 wt% NaCI

the capping agent, if any. Moreover, it was experimentally found that

dispersed in brine

the hydrodynamic diameter of the NPs is less at pH higher or lower than

Carrier medium

Synthetic brine

the IEP of the NPs, which enhances their mobility in the porous medium
[89,90]. Vayssieres et al. [91] studied the impact of particle size of
ethanol
salinity
The application of NPs in EOR and the proposed recovery mechanism.

maghemite on the pH corresponding to IEP. They reported that a shift

in the IEP of the NPs toward higher pH values was observed for smaller
particle size. For example, the IEP of 12 nm maghemite particles was
pH 6.3, whereas it shifted to pH 8.4 for 3.5 nm particles. These finding
c) Neutrally wet PSNP (NWPN)
a) Lipophobic and hydrophilic

b) Hydrophobic and lipophilic

Three different polysilicon NPs

were explained by the increased number of desorbed protons at the

Hydrophobic and lipophilic

surface of small particles. Accordingly, the surface chemistry of the

particles changes with changing the particle size and the final acidity
and/or bacesity of the particle surface is subsequently influenced.
polysilicon (HLPN)
PSNP (LHPN)

PSNP (HLPN)
Hydrophilic SiO2

Holmberg et al. [92] reported that the IEP occurs at higher pH when
TiO2 particles size is less than 5 nm. This change in IEP with size was
ascribed to changes in the crystal planes which, consequently, results in
NP type

Silica

changes in the reactivity of the surface sites. Moreover, it was found

SiO2

that the pH corresponding to the IEP of silica particles shifted to higher

values upon decreasing particle size from 40 to 6 nm, which is in good
Hendraningrat and Shidong

agreement with previous studies [93].

Onyekonwu et al. [55]

Shahrabadi et al. [64]

On the other hand, several types of NPs may interact with water and
their interaction increases in an alkaline medium which influences the
Zhang et al. [65]

material structure [94]. For example, upon dispersing ZnO into the base
Yu et al. [63]

fluid, the pH of the base fluid decreases with time due to the con-
Reference

[62]

sumption of OH− anions through hydroxylation of the surface of the

Table 2

NPs [14]. Eventually, the pH might reach a value corresponding to the

IEP leading to particle agglomeration and reduction in particle mobility

4
M.S. Alnarabiji and M.M. Husein
Fig. 1. The impact of contact angle on the adsorption of (a) hydrophobic, (b) intermediate hydrophobic and (c) hydrophilic particles onto oil-water interface
(positive and negative signs indicate salt ions).
in the porous medium. These findings may explain Al-Anssari et al.’s
[49] findings where longer contact time between the nanofluid and the
rock surface led to increased wettability of rock surface as a result of NP
destabilization and adsorption onto the rock surface. Variation of the
pH upon NP interaction with the base fluid until pH value corre-
sponding to IEP is reached may also explain why a lower flow rate of a
nanofluid through a porous medium increased NP adsorption [95],
especially since a lower flow rate corresponds to longer residence time.
Nevertheless, hydrolysis of the NPs might be negligible in certain pH
range. For example, results showed that in an acidic medium, ZnO NPs
display minimum interaction with water and the pH of the base fluid
remained almost constant with aging time [14].
2.3.3. Impact of the reservoir rock surface charge
The surface charge of the reservoir rock is very sensitive to the
surrounding conditions, especially the pH [96]. For instance, the sur-
face charge of carbonate minerals, such as dolomite and calcite, vary
from positive to negative with varying pH [97,98]. Therefore, it is ex-
pected that electrostatic interactions will dominate the adsorption be-
tween the NPs and the rock surface which may negatively affect oil
production during EOR [97,98]. Bayat et al. [99] injected three dif-
ferent types of NPs; namely: SiO2, TiO2 and Al2O3, into limestone
grains. Although Al2O3 had the biggest particle size, the experimental
results showed that 91.8% of the injected Al2O3 NPs were recovered
successfully, whereas only 72.2% and 56.6% of TiO2 and SiO2, re-
spectively, could pass through the limestone grains. The high mobility
of Al2O3 in limestone was attributed to the positive charge of Al2O3
NPs, which is similar to the surface charge of the limestone grains [99].
It is also possible to increase the mobility of NP in a reservoir by in-
jecting “sacrificial agents” to neutralize attachment sites on the re-
servoir rocks, hence improve NPs delivery [100]. Alternatively, it is
possible to overcome the electrostatic attraction of the NPs to reservoir
rocks via coating the NPs either with ionic or cationic surfactant
[35,101,102]. Coated NPs will, nevertheless, have to withstand the test
of stability criteria within the reservoir environment as well as the
environmental impact of the coating material. The effect of salinity, pH
and reservoir surface charge on the mobility of different NPs is sum-
marized in Table 3.
2.3.4. Impact of the reservoir temperature
The temperature of reservoirs varies depending on their geo-
graphical location. Reservoir temperatures may reach 100 °C, on
5
Fuel 267 (2020) 117262
average, in the Middle East and as high as 130 °C in Ekofisk field in the
North Sea [103]. Reservoir temperature has a major effect on the
characteristics of the reservoir components and mineralogy as well as
the recovery efficiency. It was found, for instance, that the carbonate
rocks become more water wet with increased reservoir temperature
[104,105]. Other rock surfaces also turn more water wet upon in-
creasing the temperature [106]. The absolute value of zeta potential of
rock minerals, such as limestone, quartz, kaolinite and calcite increased
with increasing reservoir temperature and the minerals displayed
higher negative charges at the surface [107,108]. On other hand, the
increase in temperature may cause degradation and precipitation of the
surfactants [11]. Generally, NPs display higher thermal stability than
surfactants. A study of the effect of temperature on the interfacial
tension between mineral oil and water in the presence of NPs showed
that the interfacial tension decreased with increasing the system tem-
perature [39]. It is plausible that at high temperatures Brownian dif-
fusion of the NPs is increased, as predicted by Eq. (1). The NPs partition
more effectively at the water-oil interface, hence reducing the inter-
facial tension between the two phases [109]. It should be noted,
nevertheless, that more rapid Brownian diffusion may lead to NP ag-
gregation, especially at relatively high NP concentration and/or if the
particles are not effectively coated. Moreover, at high reservoir tem-
peratures, rocks which display increase in the absolute value of zeta
potential make it challenging to inject a nanofluid having NPs with
opposite surface charge. On the other hand, the surface charge of some
coated NPs decrease upon increasing the fluid temperature [110]. This
result is ascribed to the fact that coating is an exothermic process and
tendency toward desorption is experienced at higher temperatures
[110]. Chou et al. [111] studied the impact of temperature on the pH
corresponding to the IEP of thin film of TiO2. The authors reported a
decrease in the pH corresponding to IEP from 6.62 to 5.61 with
Table 3
Summary of the impact of pH, salinity and the nature of the rock surface on
hydrophilic and hydrophobic NPs.
Hydrophilic NPs Hydrophobic NPs
pH Affect the surface charge Does not affect
Salinity Affect the surface charge Does not affect
Rock reservoir Does not easily adsorb to the rock Adsorbs easily to oil-
charge surface when carrying the same wet rocks
surface charge
M.S. Alnarabiji and M.M. Husein
increasing the temperature from 5 to 55 °C.
3. NP mobility
During EOR, the flow rate and concentration of NPs in the fluid play
a crucial role in extracting the trapped oil. When the flow rate of na-
nofluid is increased, more particles will flow, which may increase
particle deposition into the pores, but also increases particle inertia to
move through the porous media. A study of TiO2 particles (~21 nm)
transport into columns packed with 275 μm ultra-pure quartz showed
that TiO2 mobility increased with increasing the flow rate and con-
centration [112]. The hydrodynamic diameter of the agglomerated NPs
in the fluid at higher flow rate varied from ~300 nm at the inlet to
1000–1200 nm at the exit of the packing. Higher flow rate can detach
adsorbed and loosely adhered particles to other particles and/or the
packing material. Moreover, high flow rates correspond to lower re-
sidence time, hence, lower adsorption [95]. In addition, the mobility of
NPs improved because there is less contact time between the core
sample and NPs at higher velocity [113–115]. Flooding is enhanced in
some regions of the reservoir if blockage of channels or pore throats
occurs in other regions [116,117]. Higher fluid velocities in zones open
to the flow help overcoming the capillary pressure trapping the oil.
Increasing the concentration of NPs, even with particles having a much
smaller size diameter than the pore throat, might cause bridging across
the pore throat which negatively impacts rock permeability, as sche-
matically shown in Fig. 2 [59,102,118]. For instance, it was found that
90% of the agglomerated particles of TiO2 NPs (~5 nm) are lost by
filtration due to the agglomeration at high concentrations [119,120].
Consequently, a slight decrease in the recovery efficiency might take
place. In contrast, another study found that at higher concentration
more blockage of the active sites on the rock surface occurs due to NP
adsorption. Particle-particle interaction between those in the suspen-
sion and those deposited forms stable network of particles building into
the nanofluid at higher NP concentration [112]. However, using SiO2
NPs of 14 nm it was found that as NP concentration increased to beyond
3 wt%, oil production declines due to pore and channel blockage [58].
Other studies postulated that combining higher flow rate with higher
concentration of particles ensures sufficiently high hydrodynamic force,
which breaks up the aggregates and/or detaches the adsorbed/de-
posited NPs [116,117]. Yu et al. [121] investigated the effect of initial
permeability of sandstone core on core plugging and permeability al-
teration upon SiO2 nanofluid flooding. The nanofluid consisted of
11 nm spherical SiO2 NPs dispersed into 2.0 wt% NaCl aqueous solu-
tion. Two cores of 33 mD and 57.6 mD were tested. Results showed that
the pressure drop across the core was marginally influenced, suggesting
Fig. 2. 2-D Schematic diagram of vertical section of a pore shows pore throat blogging by NPs due to (a) size exclusion and (b) bridging at high NP concentration
resulting in less oil recovery.
6
Fuel 267 (2020) 117262
that no major core plugging or permeability alteration took place, likely
because the NP size was much smaller than the pore throat of the core
in both cases.
Apart from the blockage of pores and channels, Binks et al. [122]
concluded that coated SiO2 NPs with 20–50 nm and intermediate hy-
drophobicity, as a result of dichlorodimethylsilane coating, lead to
emulsion inversion from o/w to w/o upon increasing particle con-
centration [122]. To the best of our knowledge, the probability of
emulsion inversion upon increasing the concentration of NPs, during
coreflooding experiment in EOR, has not been addressed in the litera-
ture. It is noteworthy, that in water wet formation if the total surface of
the porous medium is covered with hydrophilic NPs, higher percentage
of water becomes immobile. Subsequently, less channel space would be
available for the unbound fluid to flow, which in turn mandates higher
pressure and injectivity issues. However, when using hydrophobic NPs
such as MWCNT the injectivity issues may be reduced.
The effect of rock surface properties on NP adsorption and mobility,
was investigated by injecting SiO2 nanofluid of 10–30 nm into a porous
medium consisting of alternating packing material: sand, a mixture of
kaolinite, followed by sand [95]. Results showed that NP adsorption
increased significantly when kaolinite was introduced. The increase in
NP adsorption was attributed to the increase in the surface area of the
porous medium upon introducing kaolinite. We also believe that the
lower zeta potential of the kaolinite (-18 mV as opposed to –22 mV for
sand) contributes to less electrostatic repulsion, hence more adsorption
of the SiO2 NPs having zeta potential of −4 mV.
4. Mechanisms through which NPs promote EOR
Few mechanisms were proposed to explain oil mobility from the
pores and channels of the rocks when nanofluids are used as EOR
agents. In addition to major mechanisms such as reduction of interfacial
tension, increment in viscosity, alteration of the disjoining pressure and
wettability modification [123], emulsion formation and flow confine-
ment can influence oil production.
4.1. Reduction of the interfacial tension
Reducing the interfacial tension is one of the main mechanisms in
enhancing oil recovery at the microscopic level [124,125]. A study
showed that increasing NP concentration is proportional to the reduc-
tion of interfacial tension between oil and water [126]. Nevertheless,
recent work by Wei et al. [82] showed that increasing the concentration
of nanocellulose beyond 0.8 wt% did not significantly decrease the
interfacial tension. In a similar fashion to surfactants, once the interface
M.S. Alnarabiji and M.M. Husein
between the oil and the water is fully occupied by NPs, further increase
in the concentration had no impact on the interfacial tension [36,38].
On the other hand, Reincke et al. [127] showed that the number of
entrapped coated NPs, on oil-water interface, increases and interfacial
tension decreases with decreasing the NP surface charge density.
Nevertheless, NPs entrapped at the interface must retain a certain
electrostatic repulsive to prevent irreversible aggregation of the NPs
[128]. Accordingly, high surface charge density is important for the
stability of the nanofluid, however might negatively influence IFT by
limiting the number of NPs accommodated at the interface.
4.2. Increment in viscosity
As stated earlier, NPs tend to form a thin film at the water front
during water flooding [38,109,129–131]. This kind of structuring re-
sults in higher local viscosity at the water-oil interface due to increased
number of NPs per unit volume of the interfacial region. Hence, higher
mobility ratio is achieved. This type of structuring assists in the mac-
roscopic sweep of the oil in a more “piston-like” displacement, as shown
in Fig. 3 [14].
Nanotechnology can also be used to enhance recovery efficiency by
increasing the viscosity of the displacing fluid via application of electric
or magnetic field in the presence of NPs with specific properties
[132–135]. When the applied field is electric field then this phenomena
is termed the electrorheological (ER) effect. ER effect is defined as the
effect that causes the viscosity of the suspension to increase due to the
formation of fibrillated network upon reorienting polarized molecules
along the direction of the applied field. Mainly, two dynamic processes
occur in ER fluid, as shown in Fig. 4. Firstly, polarization of particles
under the effect of the electric field. Secondly, particle alignment along
the direction of this field [136]. Interfacial polarization plays a crucial
role in producing a large amount of surface charges [136]. Irradiation
of zinc oxide nanocrystals (ZnO-NCs) suspended in a hydrosol with
electromagnetic waves during EOR stage increased their recovery effi-
ciency due to associated increase in fluid viscosity [14].
On the other hand, magnetorheological (MR) fluids are mainly
dispersions of soft magnetic particles, i.e. materials that can be easily
magnetized and demagnetize, in a carrier oil. Oil is used since it has
high viscosity and low relative emissivity, which prevent interparticle
magnetic forces from aggregating the NPs under the influence of the
magnetic field. Hence, only an increase in the viscosity of the organosol
is experienced. It is important to note that Brownian motion still
dominates over magnetic forces for ferrofluids, i.e. fluids with magnetic
NPs in the size range of 10 nm. Subsequently, a ferrofluid does not
portray significant change in viscosity when exposed to a magnetic field
[137]. Following the same logic, it can be argued that applying mag-
netic NPs might not be feasible for EOR for low viscosity base-fluid such
as water. Nevertheless, Linhardt et al. [138] prepared palladium NPs
supported onto poly (benzyl-methyl imidazolium chloride) styrene
functionalized carbon coated cobalt NPs, as magnetic nanobeads, for
Fig. 3. Schematic diagram of displacement differences for an oil droplet on a pore wall by (a) brine and (b) the self-assembly of NPs in the fluid on the interface of
nanofluid and crude oil. The flow direction is indicated by a red arrow [14]. (For interpretation of the references to colour in this figure legend, the reader is referred
to the web version of this article.)
7
Fuel 267 (2020) 117262
alkene hydrogenation. It was found that the catalyst was able to resist
agglomeration from the low viscosity reaction mixture for few minutes,
even when as strong as 1.2 T neodymium-based magnet was applied.
Moreover, Wang et al. [139] showed that 3-aminopropyltriethoxysilane
coated monodispersed Fe3O4 NP-based MR fluid with particle size of
8.4 ± 2.1 nm exhibited typical MR effects, with increased viscosity
depending on the applied magnetic field strength.
4.3. Alteration of the disjoining pressure
The spreading of NPs suspended in base fluid is different from the
spreading of the base fluid or liquids without NPs [140]. Nikolov et al.
[141] investigated the interaction of solid-nanofluid-oil system and
observed the self-structuring of the NPs due to their adsorption at the
interface between the solid and the oil forming a thin film, as shown in
Fig. 5. The resultant microstructure induced excess pressure at the
wedge-film region. The excess pressure, or the structural disjoining
pressure, displayed an oscillatory exponential decay with film thick-
ness, with both decay factor and period of oscillation equal to the ef-
fective diameter of the NPs [142]. However, below the effective dia-
meter of NPs, other disjoining pressure forces, such as electrostatic, van
der Waals, and solvation forces dominate [141–143]. The rate of na-
nofluidic film spreading is a function of NP concertation and the volume
of the oil droplet [144]. Moreover, the inner line (at the boundary
where the spreading edge of the oil-solid interface and the nanofluid
film meet as demonstrated in Fig. 5) is not observed in fluids without
NPs. Hence, the speed of the inner contact is enhanced as NP con-
centration increases and decreases with the decline in the drop volume
[144]. Alteration of the disjoining pressure helps mobilizing oil at the
microscopic level.
4.4. Wettability alteration
Many studies reported improvement in EOR using nanofluids via
wettability modification [57,145–147]. As stated earlier, several para-
meters such as reservoir pH, reservoir rock surface charge, salinity, NP
concentration and NP surface charge density, control NP adsorption to
the rock surface. Such adsorption, consequently, alters rock wettability.
Mohammed et al. [148] publish a comprehensive review on reservoir
wettability alteration via different routes; including NP use. Maghzi
et al. [58] achieved superhydrophilic surfaces using 14 nm SiO2 NPs
and decreased the contact angle of water over aged glass from 100 to 0°.
An investigation was performed on the influence of the disjoining
pressure of nanofilms on wettability alteration through injecting poly-
meric nanofluid into sintered glass-beads pack [65]. The authors used a
high resolution X-ray microtomography (micro-CT) to visualize brine
and oil distribution before and after nanofluid flooding. It was found
that wettability alteration took place via structural disjoining pressure
when a flooding experiment was performed with the nanofluid fol-
lowing brine injection. It is noteworthy that wettability alteration can
M.S. Alnarabiji and M.M. Husein Fuel 267 (2020) 117262

Fig. 4. Schematic diagram showing a ZnO nanofluid into a reservoir channel (a) before, (b) right when electrical field, E, is applied and (c) after sufficient time [14].

Fig. 5. Photograph and schematic diagram representing the inner and outer contact lines during the self-structuring of the NPs at the solid surface [144].

be enhanced by increasing nanofluid salinity, which accelerates the
precipitation of NPs onto rock surface [49]. Roustaei et al. [149]
showed that the recovery efficiency was enhanced when modified silica
NPs were injected into water-wet core thus reducing the hydrophilcity
of the core sample.
4.5. In situ formation of Pickering emulsion
Pickering emulsion is a type of complex system that forms by means
of cohesive adsorption of NPs at the oil-water interface forming a dense
monolayer or multilayer film. The film surrounds the dispersed droplets
and, subsequently inhibits their coalescence. Pickering emulsions can
also form through particles-particles interactions which lead to 3-D
complex network into the continuous phase surrounding the dispersed
droplets [150]. These emulsions have been extensively reviewed in the
literature [150–154]. Natural particles such as clays as well as syn-
thesized particles can act as emulsifiers [155–163]. Pickering emulsion
may display high stability under the harsh reservoir conditions
compared with surfactant stabilized emulsions [164] owing to the ir-
reversible adsorption of the particles at the interface [165,166]. The
particles are capable of stabilizing both o/w and w/o emulsions de-
pending on particle wettability [122,150,167]. More recently, the in
situ formation of Pickering emulsion during EOR experimental process
started to gain growing attention [60,168]. The in situ formation of this
type of emulsion results from snap-off of oil droplets into nanofluids
[169,170].The viscosity of the w/o emulsions is highly dependent on
temperature and the water fraction in the emulsion. For instance, w/o
emulsions increased the viscosity of the base fluid from a few hundred
mPa.s to ~100,000 mPa.s [151,171–173]. When forming within re-
servoirs, w/o emulsions confine the flow in highly permeable zones,
which forces the injected fluid into lower permeability zones leading to
more effective recovery of entrapped oil. Nevertheless, the probability
of in situ formation of Pickering emulsions during core flooding has not
received much attention in the literature.
The three phase contact angle (Θ) is a critical parameter for the
formation of Pickering emulsions [174]. As demonstrated in Fig. 1, this

8
M.S. Alnarabiji and M.M. Husein Fuel 267 (2020) 117262

Very hydrophobic and hydrophilic particles are better to stabilize emulsions rather than
angle determines the location of the adsorbed particles at the interface.

Emulsion type changes with changing volume fraction of water, from w/o to o/w, with
hydrophobicity of SiO2 at fixed air–water ratio or by changing air–water ratio at constant
Only intermediate hydrophobicity SiO2 were able to invert emulsion from o/w to w/o by

Inversion from air/water to water/air dispersions can be achieved by either changing the
Hydrophilic and hydrophobic SiO2 nanoparticles are able to form o/w and w/o emulsion
The maximum stability of Pickering emulsions was reported for Θ far

As the size of the nanoparticles decreases, the droplet size of emulsion dresses and the
from 90°. Such contact angles correspond to the highest adsorption of

When both hydrophilic and hydrophobic SiO2 were used, independently, emulsion
the particles into one of the phases [175]. Several fundamental studies
(summarized in Table 4) showed that NP wettability dictate the type of
emulsion formed [175,176]. For instance, hydrophilic NPs (Θ < 90°)

Double inversion is not possible for single chain cationic surfactants.

disperse mainly in hydrophilic phases, enabling the formation of o/w
emulsions and vice versa. On other hand, it was reported that the po-
larity of the oil can play pivotal role in determining emulsion type.
When partially hydrophobic SiO2 NPs (5–30 nm coated with di-

Emulsion inversion from o/w to w/o then back to o/w.

chlorodimethylsilane) were used, both o/w and w/o emulsions formed

Emulsion inversion from o/w to w/o and vice versa.

upon mixing non-polar and polar oils, respectively, with water [177].
As evident from the previous example, controlling the surface nature of
the NPs is pivotal. Efforts show that control of the NP surface wett-

intermediate hydrophobic particles.

ability can be accomplished through chemical or physical modifications

inversion occurred at 0.7 vol fraction.

of the surface. Physical modification involves decorating the surface of

increasing particles concentration.

NPs with surfactants [178–180], whereas chemical treatment involves
grafting a polymer chain onto the NPs [181–185]. Extensive review of

apparent viscosity increases.

any type of particles.
both methods of modification and the role of the modified particles in
stabilizing o/w emulsions was presented by Arab et al. [164].

particle wettability.
5. Conclusions and future prospects

respectively.
Findings
Applying nanofluids for EOR is a promising field. The high tem-

•
•
perature of reservoirs may be advantageous for nanofluid injection,
contrary to many surfactant and polymer injection processes. Moreover,

Vary weight fraction of one of particles type at

Vary length of cationic surfactant chain (8 and

injecting bare particles, whenever sufficiently dispersed, reduces the

Varying volume fraction between oil and

potential impact of the harsh reservoir environment on the coating

Changing the wettability of particles

material. Several types of NPs were successfully used to promote EOR.
However, SiO2 NPs have been the most widely used owning to their
high aqueous stability, ease of surface modification through physical
fix total particle concentration

Changing SDS concentration

and chemical methods, and, above all, their environmentally benign
chemical nature.

Particle wettability
Particle concentration
Vary volume fraction

Several parameters should be taken into consideration when NPs are

Air-water ratio
utilized in EOR. NPs with narrow and wide size distribution behave
differently at the oil-water interface. Therefore, reliable ways of mea-

Particle size
12 carbon)
Conditions

water
suring NP size distribution under reservoir conditions should be ex-
plored. Aggregation and retention of the hydrophilic NPs increase with
•
•
•
•
the increase of reservoir salinity, whereas, salinity has lower impact on
hydrophobic NPs. When it comes to surface charge, IEP of NPs is a key
parameter that should be carefully determined and managed in order to
Dodecane-water

Decane-in-brine
Cyclic silicone
Toluene-water

Toluene-water

avoid zero charged particles. The pH corresponding to IEP of several

Paraffin-water

materials changes with temperature and increases with decreasing

Air-water
oil–water

particle size. Correlating aging time of NPs in the reservoir with the pH
Phases
Fundamental studies on the role of nanomaterials in emulsion inversion.

of the formation is an important parameter which deserves more at-

NA

tention. NPs having the same surface charge as the rock surface should
Layered double hydroxide (LDH) + SDS
SiO2 (hydrophilic) + cationic surfactant

be selected in order to avoid high adsorption and ensure effective NP

mobility within the pores. Moreover, higher surface charge density of
(intermediate hydrophobicity)

the NPs ensures more stable hydrosol. Nevertheless, it may negatively

impact IFT. Reducing IFT through the use of nanofluids may not be
advantageous beyond certain NP content, in a similar fashion to sur-
factants. Higher flow rates of the nanofluid leads to higher NP mobility.
(hydrophobic)

(hydrophobic)

(hydrophobic)
(hydrophilic)

(hydrophilic)

(hydrophilic)

SiO2 (hydrophilic)

SiO2 (hydrophilic)

SiO2 (hydrophilic)

Recent studies have demonstrated the ability to manipulate the visc-

osity of smart, stimuli-responsive nanofluids by means of external
Nanomaterial

electromagnetic field. These fluids may be optimized to reduce the

overall energy required to inject the fluid, while maximizing oil pro-
SiO2
SiO2
SiO2
SiO2
SiO2
SiO2
SiO2

ductivity.
Majority of the NPs investigated for advancing EOR as well as other
Binks and Murakami [187]
Binks and Rodrigues [186]
Binks and Lumsdon [167]

Binks and Lumsdon [150]

Binks and Lumsdon [176]

applications are synthetic, which drives the cost higher, especially for
large-scale application. In addition, synthetic NPs may have adverse
environmental impact. Therefore, more attention should be paid to
Wang et al. [188]
Binks et al. [122]

Kim et al. [70]

naturally occurring NPs, e.g. nanocellulose and nanoclay.

References

Declaration of Competing Interest

Table 4

The authors declare that they have no known competing financial

9
M.S. Alnarabiji and M.M. Husein
interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.
Acknowledgment
This work was supported by Universiti Teknologi PETRONAS (UTP),
Malaysia.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://
doi.org/10.1016/j.fuel.2020.117262.
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