Yanfeng He1,2,3, Kaili Liao2,3, Jinmei Bai2,3, Lipei Fu2,3, Qianli Ma2, Xiang Zhang2, Zhangkun Ren2, Weiyang Wang1. 1. Key Laboratory of Unconventional Oil & Gas Development (China University of Petroleum (East China)), Ministry of Education, Qingdao 266580, P. R. China. 2. School of Petroleum Engineering, Changzhou University, Changzhou 213164, China. 3. Jiangsu Key Laboratory of Oil & Gas Storage and Transportation Technology, Changzhou University, Changzhou 213164, China.
Abstract
The composite flooding system composed of a surfactant and nanoparticles has shown great application potential in enhancing oil recovery. However, at present, these research studies are mainly focused on anionic surfactants. Relatively speaking, alkanolamide (CDEA), a nonionic surfactant, has the characteristics of a small adsorption amount on the rock surface, no cloud point, good temperature resistance, and good salt resistance. However, to the best of our best knowledge, there is no research report on the composite flooding system composed of CDEA and nanoparticles. Therefore, the surfactant/nanoparticle (S/NP) flooding system based on CDEA and nano-SiO2 was studied in this paper. The S/NP flooding system (0.1% CDEA + 0.05% SiO2) was constructed based on the performance in reducing the oil-water interfacial tension (IFT) and the stability of the composite system. The IFT between the S/NP flooding system and the crude oil can reach ultra-low values (3 × 10-3 mN/m), and there is no obvious sedimentation within 72 h. The sandpack flood tests show that the oil recovery rate is increased by 16.8% compared with water flooding and finally reaches 58.2%. Based on micromodel flooding tests, the mechanisms of the S/NP flooding system are studied as follows: the synergistic effect of nanoparticles and surfactants can re-enforce its oil-water interface performance and improve the oil displacement efficiency and the Jamin effect of emulsified oil droplets, combined with the thickening property and retention plugging of nanoparticles, improves the sweep efficiency. As the surfactant and nanoparticle used in this study are commercially available industrial products, the research results have important guiding significance for promoting the industrial application of surfactant/nanoparticle composite flooding technology.
The composite flooding system composed of a surfactant and nanoparticles has shown great application potential in enhancing oil recovery. However, at present, these research studies are mainly focused on anionic surfactants. Relatively speaking, alkanolamide (CDEA), a nonionic surfactant, has the characteristics of a small adsorption amount on the rock surface, no cloud point, good temperature resistance, and good salt resistance. However, to the best of our best knowledge, there is no research report on the composite flooding system composed of CDEA and nanoparticles. Therefore, the surfactant/nanoparticle (S/NP) flooding system based on CDEA and nano-SiO2 was studied in this paper. The S/NP flooding system (0.1% CDEA + 0.05% SiO2) was constructed based on the performance in reducing the oil-water interfacial tension (IFT) and the stability of the composite system. The IFT between the S/NP flooding system and the crude oil can reach ultra-low values (3 × 10-3 mN/m), and there is no obvious sedimentation within 72 h. The sandpack flood tests show that the oil recovery rate is increased by 16.8% compared with water flooding and finally reaches 58.2%. Based on micromodel flooding tests, the mechanisms of the S/NP flooding system are studied as follows: the synergistic effect of nanoparticles and surfactants can re-enforce its oil-water interface performance and improve the oil displacement efficiency and the Jamin effect of emulsified oil droplets, combined with the thickening property and retention plugging of nanoparticles, improves the sweep efficiency. As the surfactant and nanoparticle used in this study are commercially available industrial products, the research results have important guiding significance for promoting the industrial application of surfactant/nanoparticle composite flooding technology.
Petroleum is a kind of
nonrenewable resource, but with the rapid
development of economy and technology, the world’s energy demand
is constantly increasing.[1,2] This requires not only
the increase in the output of crude oil but also further improvement
in the oil production efficiency, and enhancing oil recovery (abbreviated
as EOR) has also become an important strategy for energy development
in almost all countries. Among all the EOR technologies, chemical
flooding is an effective method. Surfactant flooding can significantly
improve oil washing efficiency, which is an important chemical flooding
technology.[3−6]Anionic surfactants (such as petroleum sulfonate, alkylbenzene
sulfonate, olefin sulfonate, etc.) are widely used due to their advantages
of less adsorption loss, high oil–water interfacial activity,
and good temperature resistance.[7−9] In recent years, with the rise
of nanotechnology, surfactant/nanoparticle composite flooding technology
has been carried out for different kinds of anionic surfactants. Zhu
et al. studied the oil–water interfacial properties of nano-silica
(SiO2), modified nano-silica (M-SiO2), and petroleum
sulfonate (PS), and the results showed that the PS/SiO2 composite system could reduce the oil–water interfacial tension
(IFT) to 0.01 mN/m, while it is 0.001 mN/m for the PS/M-SiO2 composite system. The results indicate that the IFT can be further
reduced by the combination of the nanoparticles and surfactant. It
is pointed out that the mechanism lies in the complementary adsorption
of SiO2 nanoparticles and PS on the oil–water interface,
which enhances the thickness and mechanical strength of the interface
film.[10] Arab et al. comparatively studied
the oil displacement performance of sodium alkane sulfonate, modified
nano-SiO2 dispersion, and their composite system. The results
showed that the final recovery rate of the S/NP flooding system was
48%, which was significantly higher than that of pure surfactant flooding
(16%) or pure nanoparticule flooding (36%).[11] Suleimanov et al. pointed out that the oil recovery rate of the
S/NP composite system based on nonferrous metal nanoparticles with
a particle size of 70–150 nm and sulphanole-alkyl aryl sodium
sulphonate was 4.7 times that of water flooding and 1.5 times that
of surfactant flooding. They claimed that this can be attributed to
the decrease in oil–water interfacial tension and the increase
in oil displacement viscosity.[12] In addition,
Xu et al. studied the effect of nano-SiO2 on the performance
of the commercial anionic surfactant KD. The results showed that the
dosage of nano-SiO2 had a significant effect. Adding an
appropriate dosage of nano-SiO2 could further reduce the
interfacial tension, improve the temperature resistance, and also
improve the stability of its emulsion. For the ultra-low IFT nanofluid
system (0.05% KD + 0.01% SiO2), the recovery rate can be
increased by 21.12%, and the injection pressure can also be reduced
by nearly 50%.[13]However, the anionic
surfactants have the disadvantages of poor
salt tolerance and high critical micelle concentration, and a large
number of pollutants will be emitted during the production and processing
of these surfactants, which is harmful to the environment.[14,15] In contrast, the nonionic surfactant has good salt tolerance, low
critical micelle concentration, low influence by strong acid and strong
base, high stability, and good compatibility with other surfactants.[16−18] Therefore, some scholars have carried out the research on the composite
flooding technology of nonionic surfactants and nanoparticles. Zhao
et al. used a nonionic surfactant (Triton X-100) as a dispersant for
nano-silica and studied the properties of the composite system. They
pointed out that the composite system has a synergistic effect in
enhancing the system’s ability to peel off oil droplets and
changing the wetting performance. The imbibition experiment showed
that the recovery rate of the Triton X-100/SiO2 composite
system was twice that of Triton X-100.[19] Zhong et al. studied the S/NP composite system based on polyethoxylated
nonionic surfactants and hydrophilic silica nanoparticles and reached
the same conclusions.[20]Alkanolamide
is a kind of nonionic surfactant with good biodegradability,
low pollution, low price, environmental protection, and excellent
performance. In chemical flooding, its advantages are reflected in
the following aspects: excellent oil–water interfacial performance;
low adsorption capacity on the rock surface, which can reduce the
drug consumption in surfactant flooding; no cloud point, which makes
it have good temperature resistance; less affected by ions; and good
salt resistance.[21−26] Therefore, alkanolamide is an ideal surfactant for chemical flooding.
Freitas et al. studied the interfacial properties of the S/NP composite
system based on aliphatic diethanolamide and mesoporoussilica, and
the results indicated that the surfactant could be adsorbed on the
surface of nanoparticles, and the oil–water IFT could be reduced
under their synergistic effect. This study shows that the alkanolamide
has the potential to construct a S/NP composite flooding system with
nanoparticles.[27]To the best of our
best knowledge, there is no research report
on the composite flooding system based on alkanolamide and nanoparticles.
Therefore, nano-silica was added into alkanolamide solution in this
paper to construct a stable S/NP composite flooding system. The oil–water
interfacial performance, dispersion stability, oil displacement performance,
and microscopic displacement mechanism were systematically studied.
Because the alkanolamide used in this study is a commercial product,
the experimental results have important practical significance for
the promotion of surfactant/nanoparticle composite oil displacement
technology.
Results and Discussion
IFT between
Crude Oil and Flooding Solution
IFT
between Crude Oil and CDEA Solution
The IFT between crude
oil and surfactant solution with different
mass fractions of CDEA is shown in Figure . It can be seen in Figure that for CDEA solutions with the mass fraction
of 0.03 and 0.05%, the oil droplets cannot fall off the sample tube
wall in a short time even under high-speed spinning. The IFT could
be recorded after 10 and 5 min of high-speed spinning, and the equilibrium
value was higher than 1.0 × 10–1 mN/m. When
the mass fraction of CDEA was increased to 0.1–0.3%, the IFT
decreased by an order of magnitude, reaching the order of 10–2 mN/m. It can be concluded that the CDEA mass fraction corresponding
to the order of IFT from small to large was 0.1% < 0.2% < 0.3%,
as shown in Figure (right). Therefore, the mass fraction of CDEA solution was determined
to be 0.1% in the follow-up studies. Nano-SiO2 was added
into the surfactant solution to further study the influence of nanoparticles
on oil–water interfacial tension.
Figure 1
Effect of CDEA dosage
on IFT: (left) dynamic interfacial tension
and (right) IFT at 30 min.
Effect of CDEA dosage
on IFT: (left) dynamic interfacial tension
and (right) IFT at 30 min.
IFT between Crude Oil and CDEA/SiO2 Dispersion
When nanoparticles are added into the surfactant
solution, the nanoparticles can be adsorbed on the oil–water
interface, and the surfactant and nanoparticles will have a synergistic
effect to further reduce the oil–water interfacial tension.[28−30] Therefore, nano-silica was added into CDEA solution to study the
effect of nanoparticles on the IFT between CDEA solution and crude
oil. The mass fraction of the surfactant was 0.1%, and the IFT between
the S/NP composite solution and crude oil after adding different amounts
of nano-SiO2 was measured. The results are shown in Figure .
Figure 2
Effect of the dosage
of nano-SiO2 on IFT between crude
oil and the 0.1% CDEA solution.
Effect of the dosage
of nano-SiO2 on IFT between crude
oil and the 0.1% CDEA solution.It can be seen in Figure that the IFT decreased even if only 0.001% nanoparticles
were added, indicating that adding a small amount of nanoparticles
into the CDEA solution can improve the interfacial activity. However,
the IFT did not decrease by orders of magnitude, when continuing to
increase the amount of nano-SiO2 (in the range of 0.001–0.1%).
By comparing the curves in Figure , it can be seen that when the dosage of SiO2 was 0.1 and 0.05%, their IFT was relatively lower than other dosages.
The difference between the dosage of 0.1 and 0.05% was small. Therefore,
the dosage of nano-SiO2 in the 0.1% CDEA solution was determined
to be 0.05% in the follow-up experiments.The solutions used
in the determination of the oil–water
interfacial tension in Figures and 2 were all prepared with distilled
water. However, when chemical flooding is carried out in an oilfield,
all injection fluids are prepared based on formation water. Therefore,
the S/NP dispersion (0.1% CDEA + 0.05% SiO2) was prepared
with the simulated formation water, and the IFT was measured again.
The results are shown in Figure . It can be seen in Figure that for the S/NP composite flooding system
prepared with the simulated formation water, the oil drop was pulled
off after 20 min of the IFT determination process (as shown in Figure ), and the oil–water
interfacial tension was reduced to 3 × 10–3 mN/m, reaching the state of ultra-low interfacial tension, which
shows that the surfactant/nano-SiO2 flooding system has
good oil washing ability in simulated formation water and can fully
meet the oil displacement requirements.
Figure 3
IFT between crude oil
and the 0.1% CDEA + 0.05% SiO2 dispersion prepared based
on simulated formation water.
IFT between crude oil
and the 0.1% CDEA + 0.05% SiO2 dispersion prepared based
on simulated formation water.
Suspension Stability of Nanoparticle Dispersion
Among all the nanomaterials, nano-SiO2 has always been
a research hotspot in the field of oil and gas industry. For example,
its thickening effect in the water phase makes it useful for profile
control and water shutoff, and its effect of reducing the oil–water
interfacial tension makes it useful for EOR. However, due to the influence
of van der Waals force and Brownian motion, nano-SiO2 tends
to sediment in dispersions, which limits its application in oil and
gas production. Adding a polymer or surfactant to the nano-SiO2 dispersion is a common method to improve its dispersibility
in water-based systems.[31,32]Because nano-SiO2 is insoluble in water, its dispersion is turbid; therefore,
measuring the turbidity is a common method to evaluate the stability
of nanoparticle dispersions. The more the amount of nano-SiO2 contained in the dispersion, the more turbid the dispersion and
the higher the corresponding turbidity value. With the prolongation
of the storage time, some nano-SiO2 particles will deposit,
and the turbidity of the dispersion will decrease. In other words,
if the turbidity of the nano-SiO2 dispersion is low, the
amount of nano-SiO2 in the dispersion is less. If the time
factor is taken into consideration, the relationship between turbidity
and time can be obtained. The faster the turbidity decreases, the
more the nano-SiO2 will deposit in a short time and the
more unstable the dispersion is. Therefore, the suspension stabilities
of the nanoparticle dispersions and the samples added with surfactants
were evaluated by their turbidities, and the experimental results
are shown in Figures and 5.
Figure 4
Effect of the SiO2 content
on its dispersion stability.
Figure 5
Comparison
of the stability of the nano-SiO2 dispersion
and S/NP dispersion.
Effect of the SiO2 content
on its dispersion stability.Comparison
of the stability of the nano-SiO2 dispersion
and S/NP dispersion.It can be seen in Figure that when the mass
fraction of nano-SiO2 was 0.005
and 0.01%, the initial turbidity was lower, while increasing the content
to 0.05 and 0.1% significantly increased the initial turbidity. This
indicates that the initial turbidity of the dispersion was closely
related to the content of nanoparticles, and the higher the turbidity,
the more the nanoparticles dispersed in water. In addition, the turbidity
of the four nano-SiO2 dispersions decreased with the prolonging
of the standing time. However, the decrease rate of the turbidity
of the dispersion with the mass fraction of 0.1% was the largest,
indicating that this dispersion was the most unstable. In conclusion,
considering that the dispersion needs to contain the most nano-SiO2 and have the best dispersion stability, the dispersion with
the mass fraction of 0.05% was taken as the optimal candidate.By comparing the dispersion stability of 0.1% CDEA solution, 0.05%
SiO2 dispersion, and 0.1% CDEA + 0.05% SiO2 dispersion
in Figure , the following
two conclusions can be obtained. First, the turbidity of the 0.05%
SiO2 dispersion was significantly improved by adding 0.1%
CDEA. The turbidity of the 0.1% CDEA solution was very small and can
be ignored, which indicated that the addition of the surfactant CDEA
could improve the dispersion of nano-SiO2 particles in
water. Second, comparing the ratio of the turbidities of nanoparticle
dispersion and S/NP dispersion before and after 72 h, it can be found
that the turbidity of S/NP dispersion had little changes, which indicated
that the dispersion stability of nano-SiO2 dispersion had
also been significantly improved. The reason for the abovementioned
phenomenon is that the nonionic surfactant CDEA adsorbed on the surface
of nano-SiO2, increasing the hydrodynamic radius of nano-SiO2, that is, increasing the steric hindrance effect of nanoparticles.
Therefore, the agglomeration of nanoparticles can be inhibited, thus
improving their dispersion stability. Improving the stability of the
dispersion means that more nanoparticles can be adsorbed on the oil–water
interface after being pumped from the surface to the reservoir, reducing
the interfacial tension between the oil displacement fluid and the
crude oil, so as to increase the oil displacement efficiency and ultimately
improve the crude oil recovery.
Sandpack
Flood Test
The oil displacement
performance of surfactant flooding and S/NP flooding was comparatively
studied through sandpack flood experiments. Two groups of oil displacement
experiments were carried out, in which 0.1% CDEA solution and 0.1%
CDEA + 0.05% SiO2 dispersion were injected, and the injection
amount of the chemical agent was 0.5 PV. The parameters of the sandpack
model and the results of the tests are shown in Table .
Table 1
Parameters and Results
of Sandpack
Displacement Tests
oil recovery/(%)
test no.
porosity/(%)
permeability/(10–3 μm2)
initial oil saturation/(%)
chemical
flooding system
water flooding
chemical
flooding
final recovery
1
39.8
1406
86.4
0.1% CDEA
43.6
6.6
50.2
2
42.3
1370
82.4
0.1% CDEA + 0.05% SiO2
41.4
16.8
58.2
From the results of
the oil displacement experiments in Table , it can be seen that
when 0.1% CDEA was injected, the recovery rate of surfactant flooding
increased by 6.6% compared with that of water flooding, showing that
it was difficult to effectively improve the oil recovery rate using
the surfactant alone. The reason lies in that even surfactants can
reduce the oil–water interfacial tension to an ultra-low range;
the mobility (λ = k/μ, in which λ
is the mobility of the fluid, μ is its viscosity, and k is the permeability of the fluid that flows in the porous
media) of the flooding fluid is still much greater than that of the
oil phase. Accordingly, during the flooding process, a serious fingering
phenomenon occurred, resulting in the failure of the surfactant solution
to sweep to the large remaining oil area after water flooding. This
means that the sweep efficiency of the oil displacement was low, which
led to a limited increment in the oil recovery rate.However,
the increase in oil recovery rate was 16.8% compared with
that in water flooding, when the flooding fluid of 0.1% CDEA + 0.05%
SiO2 was injected. The results can be explained by the
change law of the oil recovery, water content, and differential pressure
curves of surfactant flooding and S/NP flooding in Figure . As can be seen in the water
flooding process, oil displacement pressure experienced a first-increasing
and then-decreasing process. This is because in the process of the
injected water passing through the sandpack, a dominant channel has
been formed in the simulated porous media due to the washing effect
of the injected water, along which the injected water mainly flows.
However, in areas with higher oil saturation, less oil displacing
fluid swept, so the water flooding recovery cannot be further improved.
After the injection of the 0.5 PV chemical solution, the differential
pressure began to rise in both experiments, but the pressure of the
S/NP flooding was even greater. It can be explained from two aspects:
on one hand, the addition of nano-SiO2 into the aqueous
phase had a certain thickening effect;[33] on the other hand, some nanoparticles in the oil displacement system
stayed in the smaller pore throats through a “bridging effect”,
which could temporarily block the dominant water flow channel and
allow the displacement fluid to enter the unswept oil enrichment areas.
Compared with the surfactant flooding, the sweep efficiency of oil
displacement fluid was increased, and the increment of oil recovery
was of 10.2%. Therefore, the enhanced oil recovery effect of the S/NP
composite flooding system is better than that of surfactant flooding.
Figure 6
Comparison
of (left) surfactant flooding and (right) S/NP flooding.
Comparison
of (left) surfactant flooding and (right) S/NP flooding.
Microscopic Displacement Mechanisms
In order to study the mechanism of S/NP composite flooding to enhance
oil recovery, microscopic chemical flooding (0.1% CDEA solution and
0.1% CDEA + 0.05% SiO2 system) experiments were carried
out after water flooding. The pictures of microdisplacement experiments
of water flooding are shown in Figures and 8. As can be found, the
injected water mainly moved along the diagonal direction, and the
sweep efficiency was low. In the swept area, the oil displacement
efficiency was also low, and there was still a large amount of crude
oil remaining in the pores. The residual oil existed in the form of
island remaining oil, cylindrical residual oil, film-like residual
oil, and cluster residual oil, in which, the island remaining oil
and film-like residual oil were mainly distributed in large pores,
while cylindrical residual oil and cluster residual oil were mainly
columnar and clustered and distributed in the small channels. However,
after chemical flooding (as shown in Figure ), it can be found that both the sweep efficiency
and displacement efficiency were significantly improved.
Figure 7
Microdisplacement
pictures of water flooding: (left) water break
through the production well and (right) the end of water flooding.
Figure 8
Shapes of residual oil after water flooding.
Figure 9
Microdisplacement pictures of water flooding: (left) 0.1% CDEA
and (right) 0.1% CDEA + 0.05% SiO2.
Microdisplacement
pictures of water flooding: (left) water break
through the production well and (right) the end of water flooding.Shapes of residual oil after water flooding.Microdisplacement pictures of water flooding: (left) 0.1% CDEA
and (right) 0.1% CDEA + 0.05% SiO2.The mechanism of S/NP flooding can be explained from two aspects.
From the perspective of oil displacement efficiency, it can be explained
as follows. First, the adsorption of the surfactant contained in the
system on the oil–water interface can reduce the oil–water
interfacial tension. According to the formula of adhesion work, the
decrease in oil–water IFT means the decrease in adhesion work,
that is, oil droplets are easy to be washed off the formation surface,
which improves the oil displacement ability of the flooding fluid.
Second, the active water with low IFT can soften the interfacial film
and deform the remaining oil, as can be found at the position indicated
by the red arrow in Figure . When the oil droplets flowed with the flooding fluid and
passed through the narrow throat, some oil droplets were elongated
(as can be seen at the position indicated by the green arrow in Figure ), which was conducive
to the forward migration of oil droplets through the throat, that
is, the softening–deforming mechanism improves the oil displacement
efficiency. Third, the remaining oil was emulsified under the action
of surfactants and the formed O/W emulsion, as shown in Figure . The emulsified
oil droplets dispersed in the O/W emulsion were not easy to re-adhere
to the formation surface when flowing in the porous medium, that is,
the emulsifying–carrying mechanism improves the oil displacement
efficiency. Furthermore, the addition of nano-SiO2 into
the CDEA flooding fluid would generate competitive adsorption with
CDEA on the oil–water interface, which could further reduce
the oil–water interfacial tension, enhance the interfacial
activity of oil displacement fluid, and further strengthen the abovementioned
three oil displacement mechanisms. Therefore, the residual oil saturation
in the swept area after S/NP composite flooding was very low (as shown
in Figure ), and
the oil displacement efficiency was better than that of surfactant
flooding.
Figure 10
Softening–deforming mechanism: (a) 0, (b) 2, (c) 5, and
(d) 10 min.
Figure 11
Emulsifying–carrying mechanism.
Figure 12
Comparison of the sweep efficiency of (left) 0.1% CDEA
solution
flooding and (right) 0.1% CDEA + 0.05% SiO2 solution flooding.
Softening–deforming mechanism: (a) 0, (b) 2, (c) 5, and
(d) 10 min.Emulsifying–carrying mechanism.Comparison of the sweep efficiency of (left) 0.1% CDEA
solution
flooding and (right) 0.1% CDEA + 0.05% SiO2 solution flooding.From the perspective of oil sweep efficiency, it
can be explained
as follows. First, the emulsified oil droplets generated the Jamin
effect at the small pore throat, as shown in the yellow circle in Figure b, which increased
the resistance of the oil displacement fluid, changed the flow direction
(as can be found in the changes in the arrow direction of the red
curve in Figure a,b), and displaced the remaining oil in the untouched places. Then,
these washed oil droplets blocked other pore throats again (as shown
in the blue circle in Figure d) and changed the flow direction again (as shown in Figure c,d). The repeated
occurrence of the Jamin effect in different places like this made
the oil-displacing fluid propel to the production well more evenly
in the formation and improved the sweep efficiency. Second, the dispersion
of nano-SiO2 had a shear viscosity-increasing effect. Hence,
the viscosity of the CDEA solution was improved after adding nano-SiO2, which made it have the oil displacement effect similar to
that of a polymer, that is, reducing the water–oil mobility
ratio and increasing the sweep efficiency. Third, the nanoparticles
in the composite system gathered and blocked at the small throat through
a bridging effect, thus changing the flow direction, increasing the
flow area, and increasing the sweep efficiency of the oil displacement
fluid compared with the surfactant flooding. This phenomenon could
not be observed directly in this microscopic glass model because the
average size of the nanoparticles was 20 nm. However, during our experiments,
it was found that when the mass fraction of SiO2 in the
S/NP system was increased to 1.0%, the glass model was blocked, resulting
in the scrapping of the microscopic glass model. This phenomenon indirectly
showed that the nanoparticles could block the flow channel with a
smaller pore diameter, increase the injection pressure, and improve
the sweep efficiency.
Figure 13
Jamin effect of emulsified oil droplets changes the flow
direction:
(a) initial flow direction of the flooding fluid; (b) generated Jamin
effect changes the flow direction; (c) second Jamin effect changes
the flow direction again; and (d) third Jamin effect changes the flow
direction one more time.
Jamin effect of emulsified oil droplets changes the flow
direction:
(a) initial flow direction of the flooding fluid; (b) generated Jamin
effect changes the flow direction; (c) second Jamin effect changes
the flow direction again; and (d) third Jamin effect changes the flow
direction one more time.In conclusion, the low-interfacial
tension mechanism, the softening–deforming
mechanism, and the emulsifying–carrying mechanism of the composite
flooding system improved the oil displacement efficiency, and the
Jamin effect of the emulsified oil droplets, the thickening properties
of nanoparticles, and the bridging effect of nanoparticles increased
the sweep efficiency, thereby ultimately improving the oil recovery.
Conclusions
Nano-SiO2 and CDEA
have a synergistic effect. On one
hand, the addition of nano-SiO2 can further reduce the
oil–water interfacial tension. The IFT between the S/NP flooding
system and crude oil in the formation water situation can reach the
ultra-low state (3 × 10–3 mN/m), which makes
it suitable for chemical flooding. On the other hand, the nonionic
surfactant CDEA can be adsorbed on the surface of nano-SiO2, which can increase the steric hindrance effect, inhibit the agglomeration
of nanoparticles, and improve the dispersion stability. Also, turbidity
analysis shows that the oil displacement system does not have an obvious
sedimentation phenomenon within 72 h. Based on this, the S/NP composite
flooding system (0.1% CDEA + 0.05% SiO2) was constructed.The S/NP composite flooding system could increase the oil recovery
rate by 16.8% after water flooding. Compared with pure surfactant
flooding, the recovery factor was also increased by 10.2%, which shows
that the EOR effect of the S/NP composite flooding system was better
than that of pure surfactant flooding. Micromodel displacement experiments
showed that the EOR mechanism of the S/NP composite flooding included
two aspects. On one hand, the synergistic effect of nanoparticles
and surfactants can re-enforce its oil–water interface performance
and improve the oil displacement efficiency; on the other hand, the
direction change of liquid flow caused by the Jamin effect of emulsified
oil droplets, coupled with the thickening property and retention plugging
of nanoparticles, increased the oil displacement pressure, improved
the sweep efficiency to some extent, and ultimately enhanced the oil
recovery.
Materials and Methods
Materials
The crude oil sample was
obtained from an eastern China oilfield, with a viscosity of 353 mPa·s
at 50 °C. The surfactant of alkanolamide was purchased from Haian
Petrochemical Plant with a purity of 99%. The nanoparticles were purchased
from Shanghai Xiaoge Nano Material Company, and the average particle
size was 20 nm. Other chemicals are all of analytical grade and purchased
from Sinopharm China. The simulated formation water is composed of
Cl–, SO42–, HCO3–, Ca2+, Mg2+, Na+, and K+, and the total ion content was 10137.8
mg/L.
Methods
Determination
of IFT
The spinning
drop interfacial tension meter (Shanghai Zhongchen Digital Technology
Equipment Co., LTD., TX-500C, China) was used to determine the IFT
between the chemical flooding system (CDEA solution or CDEA/SiO2 solution) and crude oil. The temperature was 70 °C,
the spinning speed was 5000 rpm, and the oil–water density
difference was 0.14 g/cm3.Its procedures and mechanisms
are as follows: first, we determine the density of the crude oil and
the chemical solution and then use the WZS-1 Abbe refractometer to
measure the refractive index of the chemical solution; second, the
length and diameter of the oil drop in the solution are determined
using the IFT meter; when the length of the oil drop is more than
four times its diameter, the dynamic interfacial tension can be calculated
according to the following formulawhere
ω is the rotational velocity (rpm), n is the
refractive index of the water phase, D is the diameter
of the oil drop (0.0001 m), Δρ is the
density difference of the water and oil phase (g/cm3),
and σ is the oil–water interfacial tension (mN/m).
Determination of the Suspension Stability
of the Nanoparticle Dispersion
The turbidities of surfactant
solutions, nanoparticle dispersions, and surfactant/nanoparticle composite
dispersions were measured using a turbidity scanner (Shanghai Xinrui
Instruments Co., LTD, WGZ-2000AP, China) to quantify the stability
of the nano-SiO2 dispersion, and the influence of CDEA
on its dispersion was evaluated. All the solutions or dispersions
were standing for different times according to the experimental requirements.
Determination of Oil Recovery Rate by Sandpack
Flood Test
In order to study the enhanced oil recovery effect
of chemical flooding, the oil displacement experiment was carried
out using sandpack models (the length is 20 cm; the diameter is 2.5
cm). The sandpack was filled as follows: we place the sandpack vertically,
appropriate amounts of quartz sand and formation water are added each
time, and the model is shaked to make the sand compact. During the
process, we make sure that the water surface is higher than the sand
surface to prevent air from entering. The flooding experiments were
conducted as follows: we vacuum the sandpack, inject the simulated
formation water at the rate of 0.5 mL/min to saturate the sandpack,
and then calculate the permeability and porosity; crude oil is injected
to saturate the sandpack until the water content of the effluent was
less than 2% and then the initial oil saturation is calculated; simulated
formation water is injected for water flooding until the water content
of the effluent was larger than 98%, surfactant solution or S/NP dispersion
is injected for chemical flooding (the injected volume was 0.5 PV),
and then, the subsequent water flooding was carried out until the
water content was 98%; and the oil recovery rates of water flooding
and chemical flooding and the final recovery rate were calculated.
Micromodel Displacement Experiment
The
microdisplacement glass model was hydrophilic and its size was
30 mm × 30 mm. The process of the oil displacement experiment
is as follows: the micromodel is vacuumed, saturated with the simulated
formation water, and saturated with crude oil at the formation temperature,
and the glass model is aged for 24 h; we inject the simulated formation
water or chemical solution, which stained with eosin at the rate of
2 μL/min to conduct the flooding test, and the video of the
displacement process was recorded.
Authors: Ahmad Nourinia; Abbas Khaksar Manshad; Seyed Reza Shadizadeh; Jagar A Ali; Stefan Iglauer; Alireza Keshavarz; Amir H Mohammadi; Muhammad Ali Journal: ACS Omega Date: 2022-07-15