IGCESH2018

Universiti Teknologi Malaysia, Johor Bahru, Malaysia 13 -15 August 2018

A REVIEW STUDY OF WETTABILITY ALTERATION BY

NANOSILICA AND POLYSILICON NANOPARTICLES

Wan Mohd Shaharizuan Mat Latif *1 , Wan Rosli Wan Sulaiman 2 and
Ahmad Kamal Idris3
1,2
Faculty of Chemical and Energy Engineering, Universiti Teknologi Malaysia,
Johor, MALAYSIA.
(E-mail: [email protected], [email protected])
3
Faculty of Engineering, Universiti Teknologi Petronas, Perak, MALAYSIA.
(E-mail: [email protected])

ABSTRACT
The applications of nanoparticles as EOR agent have attracted a lot of attention among
researchers over the past decade, including wettability alteration. Generally, the lowest
residual oil saturation is occurred in intermediate/neutrally wet, followed by water wet and
oil wet. Hence, wettability alteration is important in improving oil production rates,
production fluids ratio and reducing residual oil saturations, especially in naturally oil wet
carbonates, fractured formations and heavy-oil systems. There are several methods of
wettability alteration and the newly explored discipline is by using nanoparticles. Among
metal and non-metal nanoparticles, the best nanoparticles for wettability alteration are
nanosilica/SiO2 and three types of polysilicon nanoparticles (PSNP), which are
hydrophobic and lipophilic polysilicon nanoparticles (HLPN), lipophobic and hydrophilic
polysilicon nanoparticles (LHPN) and neutrally wet polysilicon nanoparticles (NWPN).
The wettability alteration not only affects the relative permeability and mobility ratio
towards better sweep efficiency, but it also affects the contact angle and capillary number
towards better displacement efficiency. Several factors such as nanoparticles
concentration, selection of nanoparticles size, surface modification and brine salinity were
found to be significantly associated with wettability alteration. Besides, other than NWPN,
the neutrally wet can be achieved by SiO2 and HLPN too, even at low concentration.
Key words: Wettability alteration, nanosilica, polysilicon nanoparticles, neutrally wet

INTRODUCTION
Nanoparticles possesses a significance potential in oil and gas industries as well in the
fields of EOR, reservoir characterization, exploration, drilling fluid design, well coating,
production, drilling, well completion, produced fluid treatment and tight reservoir
application [1-2]. With small size (1 to 100 nm) and high specific surface area per unit
volume, the nanoparticles can be engineered to contain specific optical, electrical or
chemical properties to perform specific functions [3]. Compared to rock’s pore size which
is much larger, the nanoparticles can easily penetrate and disperse inside porous media
with little retention on pore throat.

Nanoparticles enhance the oil recovery by several mechanisms-e.g., wettability alteration,

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gas mobility reduction, oil viscosity reduction, interfacial tension (IFT) reduction,
increasing viscosity of displacing fluid, increasing disjoining pressure gradient,
conformance control and inhibiting clay swelling [4-5]. The application of nanoparticles in
a heat transfer liquid or dispersing liquid such as brine, oil, ethanol or its mixture is called
as nanofluid. Previous studies proved that nanofluids are significantly enhanced the oil
recovery. El-Diasty and Salem (2013) [6] had flooded nanosilica fluid on Baharyia
sandstone formation, western Desert, Egypt and the result showed that nanofluid flooding
recovered 67% of original oil in place (OOIP) at breakthrough point, compared with 36%
of OOIP by water flooding. Besides, Ortega et al. (2016) [7] had proved the effectiveness
of SiO2 nanofluid in wettability alteration and IFT reduction, after experimental studied on
sandstone rock of Ben Nevis Formation, Hebron field, Canadian offshore.

Significant factors that affect nanoparticles performance in wettability alteration and other
EOR mechanisms are nanoparticles concentration, selection of nanoparticles size, surface
modification and brine salinity [8-10]. However, most of experiments in wettability
alteration were only focused on the effect of nanoparticles concentration, which will be
presented in this paper.

SILICON DIOXIDE (SiO 2) AND POLYSILICON NANOPARTICLES (PSNP)

Silicon (Si), also known as silica is the 2nd most abundant element in earth’s crust (27.7 %)
after oxygen (46.6 %) [11]. Silicon has four covalent bonding sites which can form a very
large number of potential molecules. The common form of silicon is SiO 2, which is the
principal constituent of sand and sandstone. It is slightly soluble in water with pH between
2 and 7 (~ 2 mmol/L) to form silicic acid with pK a = 9.8. The interactions of SiO 2 with
water, dissolved salts, acidic, alkaline solutions and polar compounds of crude oils are all
functions of net negative surface charges. Furthermore, each oxygen atom on SiO 2
structure has one negative charge that will be neutralized by positive cation. For example,
the negative charges of oxygen are satisfied by hydronium ion in an acidic solution.

Normally, SiO2 molecule reacts with hot or saline water to form silanol groups, which are
weak acids that capable of freeing a proton. Other than SiO 2, the silicon core can also
combine with methyl groups (-CH3) or hydroxyl group (-OH) to make Si(CH 3)4 and
Si(OH)4 respectively, where (-CH3) is used as representative hydrophobic groups and
(-OH) is used as representative hydrophilic groups. The overall hydrophobicity of SiO 2 is
controlled by the ratio of between CH3 and OH groups on interfaces [12]. Si with (-CH3)
group is known as HLPN and Si with (-OH) group is known as LHPN [13]. Besides, SiO 2
with 3-trimethoxysilyl propyl methacrylate (TPM) surface coating will produce the
neutrally wet surface wettability [14]. Additionally, it should be noted that surface
wettability of nanoparticles shows the contact angle of nanoparticles, whereas wettability
(general term) shows contact angle of porous media.

There are many advantages of nanosilica which make them receive great attention among
researchers [15]:
i. Since 99.8% of the nanosilica is SiO2, which is main component of sandstone and
quartz, nanosilica can easily be obtained and more environmentally friendly compared to
metal oxide nanoparticles.
ii. Nanosilica has good dispersion stability because its surface forces may counter balance
the gravity force easily.
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iii. Thermal, stress-strain and rheological properties of nanosilica can be tailored during
synthesis because they are strongly dependent on produced sizes and shapes.
iv. The chemical properties of nanosilica can be easily controlled by changing the surface
coating chemical. For example, the hydrophilic nanosilica can be changed to hydrophobic
by adding the lipophilic group.
v. Specific surface area (SSA) of SiO2 is barely changes even it was heated up to 650oC,
which proved that SiO2 has good thermal stability.
vi. Its price (~ $4/lb) is much cheaper compared to metal oxide nanoparticles.

WETTABILITY ALTERATION BY SiO 2 AND PSNP

To study the effect of wettability alteration by nanofluid on oil recovery, Moghaddam et
al. (2015) [16] had tested eight different nanofluids on oil wet carbonate, and the results
showed that SiO2 produced the highest oil recovery, followed by CaCO3 and TiO2. Besides,
the contact angle of oil wet carbonate decreased from 166o to 111o by SiO2 adsorption and
to 123o by CaCO3 adsorption and hence, the altered contact angle by SiO2 adsorption was
more nearer to neutrally wet (ranges from 75o to 105o). Tarek (2015) [17] also reported
that the mixture of nanofluids: SiO 2, Fe2O3 and Al2O3 recovered the highest oil recovery in
sandstone porous media compared to single nanofluid. Moreover, the experimental result
also showed that higher concentration of nanofluid mixtures produced higher oil recovery.
Additionally, Moradi et al. (2015) [18] proved that conventional water alternating gas
(WAG) in oil carbonate rock was improved by SiO 2 nanofluid, where related mechanisms
were wettability alteration, IFT reduction and increasing viscosity of displacing fluid.

Furthermore, Ogolo et al. (2012) [19] studied the oil recovery by silane treated SiO2 and
seven metal-oxide nanofluids in ethanol and brine. They displaced the injected oil with the
nanofluid and reported that silane treated SiO2 produced the highest oil recovery in ethanol
and brine, where related mechanism was wettability alteration and IFT reduction.

As previously informed, lipophobic and hydrophilic polysilicon nanoparticles (LHPN) is

used to change from oil wet to water wet or from weakly water wet to strongly water wet.
During this process, the oil relative permeability (Kro) was increased and water relative
permeability (Krw) was decreased [20]. In addition, the oil in small pores will be displaced
and the effective pore diameters for oil flow in the porous medium will be enlarged,
resulted in higher oil recovery. For example, Ju and Fan (2009) [21] had successfully
increased 17.6 % of oil recovery after injected 2 PV of LHPN on high permeability water
wet sandstone, which changed it to strongly water wet. Moreover, water of the fluids
produced from the oil well, will, in-turn, declined after the water breakthrough [22].

Other than LHPN adsorption, the wettability of oil wet rock also can be improved by
changing it to neutrally wet by neutrally wet polysilicon nanoparticles (NWPN)
adsorption, which changes it to neutrally wet. However, contrary with LHPN adsorption
which increases the Kro, the adsorption of NWPN on oil wet rock reduces the Kro [23].

On the other hand, hydrophobic and lipophilic polysilicon nanoparticles (HLPN)

adsorption (change to oil wet/strongly oil wet) is important in low permeability water wet
reservoir, where water injection either for pressure maintenance or secondary oil recovery
are very difficult to be operated. On one hand, the injection rates must be low enough to
prevent formation damages from over pressuring and inducing unwanted fracture, which
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can easily occur in low permeability reservoirs. Meanwhile, chemical injection rate should
be conducted in an optimized manner to ensure economic prospect is achieved [21].
Although some conventional stimulations such as hydraulic fracturing and acidizing are
used to improve the flow conductivity of low permeability reservoirs, the stimulations may
fail to acquire expected designation for geological complexity, which suggest the
application of HLPN [24].

Simulation studies by Ju et al. (2006) [22] also reported that HLPN adsorption
significantly increased the Krw and decreased the Kro, as wettability was altered from water
wet to oil wet. In relative permeability concept, laboratory studies by Ju and Fan (2009)
[21] reported that water effective permeability increased while water absolute permeability
decreased, which resulted in the increased of Krw by HLPN flooding.

To optimize the result of wettability alteration by SiO 2 or PSNP nanofluid, several

parameters had been analyzed by previous researchers, such as concentration of
nanoparticles, nanoparticles size, brine salinity, high pressure, high temperature and
exposure time. The effect of nanoparticles concentration, nanoparticles size and brine
salinity are described detail in next section. For other parameters, higher pressure had no
significant effect mechanism for oil wet calcite, since irreversible nanoparticles adsorption
occurred at 20 MPa [25]. On the other hand, higher temperature causes lower contact
angle of oil wet calcite which changes it to water wet. Furthermore, longer exposure time
of nanofluid to oil wet calcite surface causes higher reduction of contact angle, which
changed it to water wet state.

EFFECT OF NANOPARTICLES CONCENTRATION

Generally, higher concentration of nanoparticles will produce higher wettability alteration
effect. To study the effect of nanoparticles concentration on wettability alteration, Al-
Anssari et al. (2016) [26] had tested up to 4 wt% of SiO2 on oil wet calcite; and the result
showed that contact angle was reduced from 120 o to 60o by 1 wt% of SiO2, and further
reduced to 45o by 2 wt% of SiO2. However, the contact angle just slightly reduced beyond
3 wt% of SiO2. On the other hand, Ortega et al. (2016) [7] had proved the effectiveness of
SiO2 nanofluid in wettability alteration and IFT reduction, where optimum concentration
of SiO2 was 0.05 wt% after experimental studies on sandstone rock of Ben Nevis
Formation, Hebron field, Canadian offshore. Other experiments that studied the effect of
SiO2 and PSNP concentration effect on wettability alteration are summarized in Table 1
below.

Table 1. Effect of SiO2 and PSNP concentration on wettability alteration.

Researcher SiO2/PSNP Concentration Contact Contact
(year) (wt %) angle angle
4
 (before) (after)
Hendraningrat and SiO2 0.05 wt% 131o 110o
Torsaeter (2014) [27]
Roustaei and Bagherzadeh SiO2 0.06 wt% 146o 50o
(2015) [28]
Al-Anssari et al. (2016) [26] SiO2 1 wt% 120o 60o
2 wt% 120o 45o
Ortega et al. (2016) [7] SiO2 0.01 wt% 51.4o 37.3o
0.03 wt% 37.3o 32.4o
Zhao et al. (2018) [29] SiO2 0.1 wt% 130o 50o
Roustaei et al. (2012) [23] NWPN NA 136o 82o
Binshan et al. (2002) [24] HLPN NA 60o 158o
Onyekonwu and Ogolo (2010) HLPN 0.03 wt% 35o 90o
[30]
Shahrabadi et al. (2012) [31] HLPN 0.2 wt% 57o 85o
Ju and Fan (2009) [21] LHPN NA 120o 50o
Hendraningrat et al. (2013) [32] LHPN 0.05 wt% 54o 31o
0.1 wt% 31o 22o
Safari and Jamialahmadi (2013) LHPN 0.1 wt% 124o 30o
[33]
Safari (2014) [34] LHPN 0.1 wt% 145o 30o

As shown by Table 1 above, the optimum concentration of nanofluid for wettability

alteration is within the range of 0.05 to 0.1 wt%. It was also observed that the effect of
permeability reduction (blocking of pore network by particle aggregation) was more
dominant than wettability alteration effect when the tested concentration was beyond 0.1
wt% [32]. They reported that there was no additional of oil recovery in low permeability
core (9 mD) and less additional of oil recovery in high permeability (35 mD) core after the
tested concentration of LHPN was beyond optimum concentration. Besides, when the
concentration is beyond its optimum value, the retention and aggregation of nanoparticles
in porous media would have increases significantly [26]. Thus, the nanoparticles
concentration should be controlled properly during flooding as to achieve maximum oil
recovery without wasting the nanoparticles.

Besides, Table 1 also pointed out that there is limited study on NWPN (only one study),
even though the minimum residual oil saturation and maximum capillary number occurred
at contact angle 90o, which is neutrally wet. However, it should be noted that excess
NWPN concentration (which is beyond the optimal value) are expected to further altering
the rock wettability to water wet or oil wet, which would re-increase the residual oil
saturation back.

EFFECT OF WETTABILITY ON WAG AND FOAM FLOODING

Earlier study by Jackson et al. (1985) [35] showed that, the performance of CO2-WAG in
water wet cores was controlled by gravity override, while oil wet core was controlled by
viscous fingering. By using optimum WAG ratio, the result showed that the oil recovery
was higher in water wet after WAG as tertiary recovery, which was 20% compared to 17%
in oil wet. On the other hand, Huang and Holm (1988) [36] reported that CO 2-WAG
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produced the highest oil recovery in mixed wet (90%) after injecting 0.8 PV of WAG and
followed by 2% brine, compared to water wet (81%) and oil wet (77%). Additionally,
Farad et al. (2016) [37] showed that immiscible N2-flooding at 20% water saturation
produced oil recovery at 71.5% in mixed wet and 60% in water wet, even though gas
breakthrough was earlier in mixed wet (64 s) compared to water wet (76 s).

For foam flooding, previous studies concluded that foam is more stable in water wet
compared to oil wet and any degree of oil wet will reduce foam performance by lamellae
detaching and collapse, especially in the presence of oil [38-39]. Suffridge et al. (1989)
[40] studied the effect of Alipal CD-128 (anionic surfactant)-foam flooding on wáter wet
and oil wet Berea core (treated with Quilon C) and reported that water wet produced much
stable foam due to capability of reducing gas relative permeability. They also revealed that
detrimental effect of oil was more crucial in oil wet. Besides, Kristiansen and Holt (1992)
[41] showed that in the presence of tetralin oil, AOS-foams have higher apparent viscosity
in water wet compared oil wet, which at 45 cp compared to 6 cp. On the other hand,
Schramm and Mannhardt (1995) [42] studied the effect of Dow XS84321.05 (mixture of
anionic surfactant) in water wet and oil wet and showed that, water wet produced higher
mobility reduction factor (MRF), probably by lower surfactant adsorption on wáter wet
which influences foamability and foam performance.

CONCLUSION
As shown by Table 1, the optimum concentration of nanofluid flooding for wettability
alteration is within the range of 0.05 to 0.1 wt%, which is quite small. It was also observed
that the effect of permeability reduction (blocking of pore network by particle aggregation)
was more dominant than wettability alteration effect when the tested concentration was
beyond 0.1 wt% [32]. Besides, when the concentration is beyond its optimum value, the
retention and aggregation of nanoparticles in porous media would have increases
significantly [26].

Previous studies also showed that wettability directly affects WAG and foam flooding,
with nanoparticles concentration was found as main affecting parameter, even though
studies at neutrally wet are still limited. The fact that Alkaline-Surfactant-Gas (ASG) was
more effective than Alkaline-Surfactant-Polymer (ASP) [43-44] and foam assisted water
alternating gas (FAWAG) was better than WAG in recovering oil [45-46], hence, it is
highly anticipated that ASG and FAWAG could be improved by SiO 2 and PSNP too.
Lastly, the contribution of NWPN should be getting more attention in EOR research due to
its vast enhancing effects.

Acknowledgment: The authors are grateful to Malaysia Ministry of Education for funding
this research.

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