SPE 165283 Enhancing Oil Recovery of Low-Permeability Berea Sandstone Through Optimized Nanofluids Concentration
SPE 165283 Enhancing Oil Recovery of Low-Permeability Berea Sandstone Through Optimized Nanofluids Concentration
This paper was prepared for presentation at the S P E E nhanced Oil Recovery Conference held in K uala Lum pur, M alaysia , 2-4 July 2013.
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Abstract
Current global demand for fossil fuel such as oil is still high. This encourages oil and gas industries to improve their effort of
finding new discoveries, developing technique and maximizing recovery of their current resources including in low-
permeability reservoir. Enhanced oil recovery (EOR) is a technique to enhanced ultimate recovery. Since technology has been
continuously developed such as nanotechnology/nano-size material, EOR methods have improved. One of them is Nano-EOR
that triggered great attention in last decade. Nanoparticles may alter the reservoir fluid composition and rock-fluid properties
to assist in mobilizing trapped oil. Most of observation from lab-scale reported that it seems potentially interesting for EOR.
Since reservoir management is very essential for the success of all improved/enhanced oil recovery (IOR/EOR) methods,
optimizing nanofluids concentration is a proposed reservoir management to maximize oil recovery using Nano-EOR in this
paper. Low-permeability water-wet Berea sandstones core-plugs with porosity ranged 13-15% and permeability ranged 5-20
mD were tested. A hydrophilic silica nanoparticles with primary particle size 7 nm was employed without surface treatment.
Nanofluids with various concentration ranged 0.01 – 0.1 wt.% were synthesized with synthetic saline water for optimizing
study. The wettability alteration due to nanofluids was observed; coreflood experiment was conducted and compared its
displacement efficiency.
The results observed a range of nanofluids concentration that could maximize oil recovery in low-permeability water-wet
Berea sandstone. Although contact angle of aqueous phase decreases as nanofluids concentration increase which means easier
of oil to be released but we observed that higher concentration (e.g. 0.1 wt.%) has a tendency to block pore network and will
decrease or even without additional oil recovery.
This study provides if concentration of nanofluids has an important parameter in Nano-EOR and could be optimized to
maximize oil recovery of low-permeability water-wet Berea sandstone.
Introduction
Recent advanced technologies have exposed to improve and be a better understanding the complexity of enhanced oil recovery
(EOR) processes both current and new method such as using nanoparticles (Nano-EOR). Nanoparticles have average size less
than 100 nm. It has developed largely over the past decade and revealed its potential applications in oil and gas industries.
Nano-EOR has recently taken a great attention in a decade. Most of results from lab-scale reported that it seems potentially
interesting for future EOR.
Traditional EOR displacement mechanism focuses on three forces : capillary, viscous and gravity (Fletcher, 2010). Meanwhile
nanotechnology will focus on nano-scale forces such as disjoining force as experimentally investigated by Wasan and Nikolov
(2003); Chengara et al. (2004); and Wasan et al. (2011). Since oil recovery depends on nano-scale process (Fletcher, 2010), we
would like to bring the benefit of nanoparticles size as EOR possibility into low-permeability rocks. Fletcher (2012) mentioned
low-permeability reservoirs still have large volume of oil resources. He also mentioned the major challenges in developing
low-permeability reservoir are poor sweep efficiency, low productivity and waterflood injectivity .
Nanoparticles may alter the reservoir fluid composition and rock-fluid properties to assist in mobilizing trapped oil. In
previous study, we have observed that it could alter interfacial tension (IFT) in water-oil system and wettability. Introducing
lipophobic and hydrophilic nanoparticles (LHP) silica nanoparticles into the brine-oil system was observed to give lower IFT
and the decreased might be large enough to produce more oil (Hendraningrat et al., 2013). It may involve several
2 SPE 165283
physical/chemical interactions that can lead to efficient microscopic displacement with low residual oil saturation . Buckley
and Fan (2005) reported IFT impacts on capillary pressure, capillary number, adhesion tension, and the dimensionless time for
imbibition. The capillary number increased with decrease of IFT and consequently some residual oil is mobilized. Morrow
(1990) reported wettability has a vital role in crude oil production and determines the recovery efficiency of displacement
processes. Wettability affects both the distribution of hydrocarbon and aqueous phases within the rock matrix and dynamics of
displacement processes (Fletcher, 2012).
This study is an extended work from previous (Hendraningrat et al., 2013). We observed if LHP silica nanofluids
concentrations play an important role in Nano-EOR, especially in water-wet sandstone rocks. Although IFT and contact angle
of aqueous phase decreases as nanofluids concentration increase which means easier of oil to be released but we observed that
higher concentration (e.g. 0.1 wt.% or more) has a tendency to block pore network and will decrease or even without
additional oil recovery (Hendraningrat et al., 2012 and 2013). There is a range of nanofluids concentration that could
maximize oil recovery in low-permeability water-wet Berea sandstone. Finding optimum nanofluids concentration in low-
permeability sandstone core is a main purpose in this study as part of reservoir management to maximize oil recovery using
Nano-EOR.
Experiments
Material
A crude oil (degassed) from a field in North Sea has been employed in this study. Synthetic reservoir brine was made as base
fluid solution between sodium chloride (NaCl) 3.0 wt.% and de-ionized water. The density and viscosity were measured using
pycnometer and Brookfield rotating viscometer respectively at room condition (see Table 1).
Similar to previous study (Hendraningrat et al., 2013), a hydrophilic silica nanoparticles from Evonik Industries, with primary
particle size 7 nm was employed without surface treatment. It consists of silicon dioxide (SiO2 ) more than 99%. The LHP has
been characterized under Zeiss Supra 55 VP low vacuum Scanning Electron Microscope (SEM) with scale of 200 nm as
shown in Figure-1. It has aggregated size 40 to 60 nm dispersed in brine (Hendraningrat et al., 2013).
Fig. 1─ Nanoparticles characterization under SEM (magnification >40k times) compared with pen cap (4 cm)
To investigate optimum nanofluids concentration (in weight percentage), various concentration with narrow range from 0.01 to
0.1 wt.% were synthesized using high speed magnetic stirring and continued exposing with ultrasonicator at 40-100%
amplitude for 5 minutes. Fluid properties measurement of brine and various nanofluids concentrations at room condition are
summarized in Table 1. Introducing nanoparticles into brine decrease pH and density at range 0.01 – 0.1 wt.%.
Table 1. Fluid properties
Fluid Density, g/cm3 Viscosity, mPa.s pH Temperature, oC
Crude Oil 0.826 5.10 - 22.0
Brine, NaCl 3 wt.% 1.022 1.00 6.76 21.4
Nanofluid 0.01 wt.% 1.012 1.01 6.26 21.7
Nanofluid 0.02 wt.% 1.012 1.01 6.15 23.1
Nanofluid 0.03 wt.% 1.014 1.01 6.14 22.1
Nanofluid 0.04 wt.% 1.015 1.01 6.04 23.1
Nanofluid 0.05 wt.% 1.015 1.01 6.16 21.2
Nanofluid 0.06 wt.% 1.016 1.01 5.88 19.9
Nanofluid 0.07 wt.% 1.017 1.01 5.74 21.1
Nanofluid 0.08 wt.% 1.018 1.02 5.59 19.9
Nanofluid 0.09 wt.% 1.018 1.02 5.56 23.6
Nanofluid 0.1 wt.% 1.017 1.02 5.25 20.0
SPE 165283 3
Porous Rock
Twenty low-permeability Berea sandstone (ss) cores were tested in this study. These cores with average length 3.8 cm and
diameter 4.1 cm have been dried and cleaned before measuring their rock properties . The range of porosity and permeability
are 13-15% and 5 to 20 mD respectively. The average pore volume (PV) of tested cores is 6.7 cm3 . The measured dimension
and average petrophysical properties at initial condition are tabulated in Table 2.
Table 2. Dimensions and average petrophysical properties at initial condition
Berea Length, Diameter, Pore Volume, Helium-Porosity, Avg. Liq. Permeability,
ss # cm cm cm3 % mD
1 4.08 3.80 7.0 15.2 13
2 4.07 3.80 6.4 13.9 9
3 4.08 3.81 6.9 14.9 14
4 4.08 3.82 7.1 15.1 8
5 4.01 3.80 6.1 13.5 20
6 4.10 3.80 7.0 15.1 8
7 4.08 3.81 6.6 14.2 7
8 4.08 3.81 6.4 14.1 5
9 4.09 3.82 7.0 15.0 7
10 4.10 3.83 7.2 15.2 7
11 4.08 3.79 6.8 14.7 9
12 4.09 3.79 6.7 14.6 9
13 4.01 3.81 6.5 13.4 8
14 4.10 3.80 7.0 15.0 12
15 4.08 3.80 6.6 14.3 10
16 4.07 3.79 6.8 14.7 8
17 4.05 3.81 6.0 13.2 15
18 4.09 3.81 6.8 14.6 12
19 4.10 3.78 6.9 14.9 18
20 4.07 3.80 6.5 14.1 10
Core pore-size characterizations were conducted using scanning electron microscope (SEM) integrated with energy dispersive
X-ray spectroscopy (EDX). As shown in Fig. 2, pore-size seems at a glance dominated in range 4-7 µm for this low-
permeability of Berea sandstone. However some larger pores appear such as shown in Fig.2. Crocker et al. (1983) reported
average pore size for Berea (porosity 19.2% and permeability 302 mD) is 18 µm. Nanoparticles dispersed in fluid may
agglomerate in micron size without dispersing agent. It will be an issue in low-permeability rocks and cause formation
damage.
Low-Perm. Berea ss
4.1 cm
3.8 cm
Fig. 2─ (a) Low-Medium permeability Berea ss with its pore size morphology under SEM
Interested Area
Fig. 3─ Mineral elements analysis using EDX integrated with SEM on sister core #1
Interested
Area
interaction
between
brine/nanofl
uid and clay
may not the
main cause
Intereste of
d Area
Interested Area
Fig. 4─ Mineral elements analyses using EDX integrated with SEM on sister core #2
SPE 165283 5
where σ describes interfacial tension components of phase, indices s and l stand for solid and liquid phases, σsl represents the
interfacial tension between the two phases and θ is contact angle corresponding to the angle between vectors σl and σsl .
Fig. 5─Contact angle formation on polished synthetic silica between crude oil and Brine/nanofluids according to Young formula
4
4
4
4
7 8 9
2 18
6
1 4 6 6
5
5 5
3 13 14
16
12 19
1) Pump fluid (Exxol D60); 2) injection line; 3) Micro Pump; 4) Valve; 5) Pump Fluid in Vessel-A; 6) Piston plate; 7) Brine in Vessel-A; 8) Oil in Vessel-B;
9) Nanofluid in Vessel-C; 10) Oil line; 11) Brine/Nanofluid line; 12) Bypass Valve; 13)Hassler Core Cell; 14) Core plug inside cell; 15) Pressure gauge; 16)
Sleeve pressure; 17) connection cable; 18) Computer; 19) Accumulator
54.0
50
40.0 37.7
40 35.6
34.7
31.0
29.3 27.6
30 26.4
25.3
22.0
20
10
0
0 0.01 0.02 0.03 0.04 0.05 0.06 0.07 0.08 0.09 0.1
Fig. 7─Contact angle measurement for crude oil against brine with various nanofluids concentrations at room condition
SPE 165283 7
Fig. 8─Oil drop imaging (flipped) from Goniometry KSV CAM in crude oil-brine /nanofluids on polished synthetic silica at room condition .
The oil drop volume was in range 10-17 µL.
Coreflood Results
All twenty cores have been conducted secondary process by injecting brine for approx. 3-12 PV until surely no more oil
produced and thereby first residual oil saturation was established. In this secondary process, oil recovery factor are in the wide
range 36-81% OOIP. Then the injection was continued approx. 3-8 PV of Nano-EOR process. Figure 9 shows secondary
process during brine flooding in blue line and Nano-EOR in red line with various concentrations. In most cases, nanofluids
need first 1-2 PV to mobilize remain oil in cores.
80 %
Core #6 (Nano 0.03 wt%)
Core #7 (Nano 0.04 wt%)
Core #5 (Nano 0.03 wt%)
Core #4 (Nano 0.02 wt%)
Core #15 (Nano 0.08wt%) Core #12 (Nano 0.06 wt%)
70 % Core #10 (Nano 0.05 wt%)
Core #18 (Nano 0.09wt%)
Core #13 (Nano 0.07wt%) Core #11 (Nano 0.06 wt%)
Core #14 (Nano 0.07wt%)
Core #8 (Nano 0.04 wt%)
Core #19 (Nano 0.1wt%) Core #17 (Nano 0.09wt%)
60 % Core #3 (Nano 0.02 wt%)
Core #9 (Nano 0.05 wt%)
Core #1 (Nano 0.01 wt%)
40 %
Core #2 (Nano 0.01 wt%)
30 %
20 %
0 4 8 12 16 20 24
Pore Volume Injected
Table 5 shows tabulation of coreflood process both secondary and tertiary processes. The additional oil recovery due to Nano-
EOR surprisingly reached up to 10% points at 0.05 wt.% concentration (core #10). Nano-EOR seems also possible for mature
field with low-permeability which already has recovery factor more than 70%. Based on results of cores #5, #6, #7, #12 and
#15, Nano-EOR could increase oil recovery up to 4% points.
Green and Willhite (1998) described the effectiveness of process fluids in removing oil from rock pores at the microscopic
scale is an important aspect of any EOR process. Microscopic displacement efficiency determines the failure of success of any
EOR process. In this study, we evaluate nanofluids efficiency in displacing of remains oil at low-permeability sandstone pore-
scale using formula as follows:
where S or1 represents residual oil saturation after brine injection and S or2 represents residual oil saturation after nanofluids for
EOR.
We observed that there is no significantly an oil viscosity change before and after Nano -EOR. Hence we can assume no
volume changes associated with pressure changes and formula (2) represents also oil recovery efficiency. Figure 10 shows
displacement efficiency of twenty cores at various concentrations. Related to displacement efficiency, there are some
parameters that will be discussed such as concentration, injected PV of nanofluids and rock permeability.
The interesting nanofluids concentration is at 0.01, 0.03 and 0.05 wt.% where favorable nanofluids concentration is at 0.05
wt.% with respect to the highest displacement efficiency (25%). However economic evaluation should be studied to consider
costs, values, etc. Currently, the massive production cost of nanoparticles is still unknown. However low-cost and high volume
production of green nanofluids (health and environmental issue) would be one of the most challenging future research
directions. In addition, nanoparticles have a tendency to block pore network at higher concentration (e.g. > 0.06 wt.%) in low-
permeability Berea cores. We observed most nanoparticles aggregated at inlet cores (see Fig. 11) at higher concentration.
Meanwhile lower concentration created less aggregated nanoparticles at inlet cores (see Fig. 12).
Based on our observation, there is no direct relationship among total injected PV of nanofluids , rock permeability and
displacement efficiency. In case 0.03 wt.%, core #6 with lower permeability and injected PV than core #5, has significantly
higher displacement efficiency. In another case 0.01 wt.%, core #2 with lower permeability resulted in higher displacement
efficiency than core #1 at almost similar injected PV of nanofluids. However other cases such as 0.05 wt.% and 0.06 wt.%
show the trend of higher displacement efficiency as increase injected PV at similar rock permeability. Again, higher
permeability does not guarantee higher displacement efficiency like core #5 at 0.03 wt.% or even no additional oil recovery
such as core #19.
Table 5. O il Recovery due to Brine and Nano-EO R with various concentrations
and Displacement Efficiency at constant injection rate 0.2 cm 3 /min
Berea Oil saturation Oil Recovery Nano- Injected Oil saturation after Ultimate Oil Displacement
ss after Brine after Brine EOR PV at Nanofluids Injection Recovery after Efficiency of
# Injection (Sor1), Injection, Scenario Nano-EOR (Sor2), Nano-EOR, Nanofluids, ED
% % OOIP % % OOIP %
1 36.0 55.6 0.01 wt.% 2.7 33.8 58.2 5.9
2 53.7 36.1 0.01 wt.% 3.1 49.1 38.0 8.7
3 32.5 56.3 0.02 wt.% 3.4 30.3 59.2 6.7
4 20.2 71.3 0.02 wt.% 3.4 19.9 71.7 1.4
5 20.4 71.9 0.03 wt.% 7.2 18.4 74.6 9.6
6 19.9 72.5 0.03 wt.% 5.3 16.8 76.9 15.7
7 19.0 74.2 0.04 wt.% 3.2 17.8 75.9 6.4
8 28.8 62.2 0.04 wt.% 5.8 28.0 63.3 2.7
9 32.0 53.6 0.05 wt.% 5.4 27.1 60.6 15.1
10 28.0 60.4 0.05 wt.% 6.1 21.0 70.3 25.0
11 24.4 65.6 0.06 wt.% 7.2 22.5 68.3 7.9
12 22.3 70.0 0.06 wt.% 4.7 21.1 71.6 5.3
13 26.0 64.9 0.07 wt.% 4.6 24.4 67.0 5.9
14 29.4 61.3 0.07 wt.% 6.0 27.5 63.8 6.3
15 20.4 70.7 0.08 wt.% 4.5 19.7 71.7 3.7
16 14.8 80.8 0.08 wt.% 7.6 14.3 81.3 3.0
17 29.2 60.2 0.09 wt.% 5.0 28.7 60.9 1.7
18 23.5 68.3 0.09 wt.% 6.2 23.1 68.9 1.9
19 25.8 62.2 0.1 wt.% 2.8 25.8 62.2 0.0
20 37.8 49.0 0.1 wt.% 3.0 37.8 49.0 0.0
SPE 165283 9
#6 (8 mD, 5PV)
#9 (7 mD, 5PV)
30
#5 (20 mD, 7PV)
#7 (7 mD, 3PV)
25
20
Outlet
agg
Inlet
Outlet
Fig. 11─Nanoparticles was aggregated at inlet surface rock and less at outlet at concentration 0.06 wt.%
Inlet
agg Outlet
Inlet
Fig. 12─Nanoparticles was aggregated at inlet surface rock and less at outlet at concentration 0.03 wt.%
10 SPE 165283
Concluding remarks
Based on this experimental lab-scale study, we conclude that concentration of nanofluids has an important parameter in Nano-
EOR and could be optimized to maximize oil recovery of low-permeability water-wet Berea sandstone. Contact angle
decreases as nanofluids concentration increases and there is interesting nanofluids concentrations: 0.01, 0.03 and 0.05 wt.%
where favorable nanofluids concentration is at 0.05 wt.% with respect to the highest displacement efficiency (25%).
Nanoparticles have a tendency to block pore network at higher concentration (e.g. > 0.06 wt.%) in low-permeability Berea
cores.
In further, economic evaluation should be studied to consider costs, values, etc. Currently, the massive production cost of
nanoparticles for EOR is still unknown. However low-cost and high volume production of green nanofluids (health and
environmental issue) would be one of the most challenging future research directions.
Acknowledgments
The authors gratefully acknowledge to laboratory engineer staff, Roger Overå, who has prepared low-permeability Berea ss
core plugs and Statoil ASA which has granted a travel support. The authors also appreciate the permission granted by NTNU
to publish this paper.
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