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Keywords: The blockage produced during polymer flooding can lead to a significant decline in reservoir productivity. The
Blockage composition of the oilfield scale is very complicated, and formation mechanism and location distribution of
Composite scale blockage are unclear. In this work, the composition of the oilfield scale produced during polymer flooding was
Component analysis
analyzed by thermal gravimetric analysis (TGA), infrared spectrum analysis (FI-IR), X-ray diffraction analysis
Formation mechanism
(XRD), and scanning electron microscopy observation (SEM). The formation mechanism of the blockage was
Location distribution
studied by means of water compatibility experiment, core flooding experiment, swelling experiment, and
polymer retention experiment. The location distribution of blockage was explored by physical simulation
displacement experiment using the long sand pack tube. The results show that the oilfield scale is composed of
polymer, inorganic substances, water, and crude oil. Various components are interdependent and entangled in
the scale. After the polymer solution is injected into the formation, the “fish eye” scale and inorganic salt crystal/
polymer scale are produced in the near-injection well zone. Through scale migration and fine particle exfoliation,
there occurs the complex composite scale combined by migrated scale and fine particles as well as the newly-
generated fine particle/polymer flocculent scale. When the scale encounters with crude oil, the asphaltene
from crude oil can be adsorbed and precipitated on the scale surface, leading to the oil-wrapped composite scale.
Besides, the injected polymer can be adsorbed and captured in the oil layer, causing the decrease of the layer
permeability. With decrease of oil layer permeability, various scale is deposited and bridge-blocked in the oil
layer, causing the blockage during the polymer flooding process. After three displacement stages of water
flooding, polymer flooding, and subsequent water flooding, blockage is produced in all zones of oil layer, with
the most severe blockage in the middle zone near the injection well. The study can provide a theoretical basis for
the subsequent research on the blockage-removing fluid systems suitable for polymer flooding reservoirs.
* Corresponding author. School of Petroleum Engineering, China University of Petroleum (East China), Qingdao, 266580, PR China.
E-mail address: kangwanli@upc.edu.cn (W. Kang).
https://doi.org/10.1016/j.petrol.2020.107503
Received 17 April 2020; Received in revised form 1 June 2020; Accepted 3 June 2020
Available online 7 June 2020
0920-4105/© 2020 Elsevier B.V. All rights reserved.
F. Wang et al. Journal of Petroleum Science and Engineering 194 (2020) 107503
flooding and further promote the blockage-removing technology inductively coupled plasma mass spectrometer (Thermo Electron Corp,
development, extensive research has been done to study the blocking America) was used to detect the anion and cation composition and
causes and mechanisms during polymer flooding (Meng et al., 2011; content of the filtered injection water and formation water. The
Chen et al., 2018a; Guo, 2017). There are a number of factors contrib composition of injection water and formation water was shown in
uting to the blockage during polymer flooding. Polymer retention, Table 2. The injection water and formation water used in this paper were
including polymer adsorption which can diminish the pore diameter and simulated injection water and formation water made up of salts and
polymer capture which can block the narrow pore throats, is an inevi distilled water according to the ion content of two water sources.
table mode of blockage during polymer flooding (Liu et al., 2013;
Oulanti et al., 2009). Furthermore, the poorly dissolved polymer dry 2.2. Fourier transform infrared spectroscopy (FT-IR) analysis
powder and bacteria in the injection fluid can result in soft particle scale
blocking in the oil layer (Wood and Spark, 2000). The incompatibility Blockage structure and polymer powder structure were character
between the injection water and the formation water can lead to the ized by Fourier transform infrared spectroscopy (FT-IR) analysis, carried
blockage of inorganic salt crystal scale (Shabani et al., 2019). Moreover, out by KBr disk tablet method, using a Nexus FT-IR spectrometer
the exfoliation and migration of clay particles in the layer can further (Nicolet Inc., USA).
aggravate the blockage (Gabriel and Inamdar, 1983). For some heavy oil
reservoir, the resin and asphaltene from crude oil can be flocculated and 2.3. Thermal gravimetric analysis
deposited, forming the organic scale blockage (Khormali et al., 2018;
Wang et al., 2016). Besides, it is proved that interactions between The thermal gravimetric analysis was carried out by STA49F3
inorganic scale (such as inorganic salt scale and fine particles) and synchronal thermal analyzer (Netzsch company, Germany). With the
organic substances (such as polymer molecules and heavy hydrocarbons temperature increasing from room temperature up to 1000 � C, the oven-
from crude oil) can lead to the organic-inorganic compound scale (Chen dried scale sample was measured. With the temperature increasing from
et al., 2018a,b,c; Lu et al., 2016). Above various research mainly focuses room temperature up to 850 � C, the polymer powder sample was
on the theoretical forming mechanisms of blockage and is lack of oilfield measured. Then the relationship curves between sample weight and
practicability. So it is necessary to further study the consecutive for temperature were obtained.
mation mechanism of blockage during the whole polymer flooding
process and then clarify the location distribution of blockage in the oil 2.4. X-ray diffraction analysis
layer.
In this study, taking the blockage of the polymer flooding oil layer in X’Pert PRO X-ray diffractometer (Panalytical ICP, Holland) was used
Bohai oilfield (China) as an example, based on the analysis about genetic to characterize the blockage microstructure. The measurement condi
mechanisms of various scale and interaction mechanisms among various tions were: maximum power 3 kW, goniometer radius 135–320 mm, X-
scale, the consecutive formation mechanism of blockage during the ray tube voltage 45 KV, tube current 50 mA, minimum step length
whole polymer flooding process was summarized, and the location 0.0001� , 2θ range 0� –167� , scanning method θ/θ or 2θ/θ.
distribution of blockage in the oil layer was obtained through the
physical simulation displacement experiment. The study intends to 2.5. Micrograph measurement
provide a theoretical basis for the subsequent research on the blockage-
removing fluid systems suitable for polymer flooding reservoirs. The micrograph was observed by Hitachi S4800 (Hitachi Company,
Japan) field emission scanning electron microscopy (SEM). The sample
2. Experimental of blockage was treated by air-drying in a dryer and spray-gold.
Oilfield blocking scale and polymer dry powder were provided by The simulated injection water and simulated formation water were
Bohai oilfield (China). The polymer is a kind of commercial applicable mixed in various volume ratios (3: 7, 4: 6, 5: 5, 6: 4, and 7: 3). Then the
product (Guangya Technology Ltd, Sichuan, China). The viscosity- mixtures were sealed and heated in 65 � C thermostat water bath for 24
averaged molecular weight (Mη) of the polymer is approximately h. Whether there occurred precipitation could be observed. Meanwhile,
1800 � 104, and the density of dry powder is 1.1 g/cm3 (Zou et al., the same simulated injection water with polymer dissolved in them were
2014). The polymer structure is shown in Fig. 1. Sodium carbonate added to the simulated formation water. Then the compounding solu
(Na2CO3), sodium chloride (NaCl), sodium sulfate (Na2SO4), sodium tions were also heated in 65 � C thermostat water bath for 24 h to observe
bicarbonate (NaHCO3), calcium chloride (CaCl2), magnesium chloride the precipitation situation.
hexahydrate (MgCl2), potassium chloride (KCl), and hydrochloric acid
(HCl) were all analytical grade and purchased from Sinopharm Chemical 2.7. Core flooding experiments
Reagent Co., Ltd. (Shanghai, China). The oil used in this study was
dehydrated crude oil from Bohai oilfield (China). The properties of According to the actual development condition of Bohai oilfield, the
crude oil are shown in Table 1. The injection water and formation water core flooding tests were carried out using the one-dimensional homo
provided by Bohai oilfield were filtered. Then the ICP MS-2030 geneous cores. The schematic of core flooding tests is shown in Fig. 2.
The experimental setup consisted of constant flow pump, three stirring
vessels, a core gripper and the pressure transducers connected to a
computer for continuous recording of the inlet pressure. The core
flooding experiments included polymer retention experiment, inorganic
salt crystal/polymer scale blockage experiment, and oil-wrapped scale
blockage experiment. All the core flooding tests were conducted at the
reservoir temperature of 65 � C. The size of the homogeneous cores is
ϕ25 � 300 mm.
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F. Wang et al. Journal of Petroleum Science and Engineering 194 (2020) 107503
Table 1
Properties of dehydrated crude oil from Bohai oilfield.
Overground Density (g/cm3) Viscosity (mPa⋅s) Freezing point Wax content Resin content Asphaltene content
Undergroud Degas ( C)
�
(%) (%) (%)
Table 2
Bohai oilfield formation water and injection water.
Composition Cation (mg/L) Anion (mg/L) Total (mg/L)
Formation water 3183.2 128.3 26.7 4847.8 147.1 241.3 67.1 8641.5
Injection water 2620.7 235.8 58.2 4506.6 11.5 45.1 187.9 7665.8
Fig. 2. Schematic of core flooding experiments. 2.7.3. Oil-wrapped scale blockage experiment
The oil-wrapped scale blockage experiment was also carried out with
permeability were used to measure the effects of polymer retention on the R5 core. After being saturated with formation water, the core was
the core permeability. The four cores were labeled as R1, R2, R3, and R4. injected with 2 PV polymer/formation water solution at the rate of 0.1
The permeability data of the cores are shown in Table 3. mL/min. Then 5 PV crude oil was injected as experimental group. The
The experiment was conducted in the following process: injection pressure data was real-time recorded. After the experimental
group measurement was finished, the core was cleaned, and then for
a. The polymer solution was prepared by polymer dry powder and mation water saturation step and 2 PV polymer/formation water in
formation water. The concentration of the polymer solution was jection step were repeated. Then 5 PV polymer/distilled water solution
2000 mg/L. with the same viscosity as crude oil in experimental group was injected
b. The porosity of core was measured using weight method. as contrast group. The injection pressure data was real-time recorded.
c. The formation water was injected into the core at injection rates of
0.2 mL/min, 0.4 mL/min, and 0.6 mL/min respectively, and the 2.8. Sand pack tube flooding experiment
stable injection pressures were recorded. The core permeability was
calculated according to Darcy’s law, and the initial permeability k0 The schematic of the sand pack tube flooding experiment is the same
was obtained by the average of three testing values. as the core flooding experiments. The sand pack tube was made of quartz
d. At the injection rate of 0.2 mL/min, the core was injected with 10 PV sand combined of 40 mesh (90%) and 150 mesh (10%). The length of the
polymer solution, and then the formation water was injected until sand pack tube was 100 cm while the cross-sectional diameter was 2.5
there was no polymer solution produced. cm. The sand pack tube was averagely divided into four zones, and the
e. The core permeability kt was calculated again using the same distribution of four zones (I,II,III,Ⅳ) and four pressure measuring
method. points (P1, P2, P3, P4) are shown in Fig. 2. The average permeability of
f. Change different cores, and repeat the above experimental steps. sand pack tube was 253.38 � 10 3 μm2 and the degree of porosity was
g. Permeability damage rate was calculated by the following formula: 27.95%, which were consistent with the oil layer characteristics. The
ðk0 kt Þ flooding experiment was conducted at the reservoir temperature of 65
Permeability damage rate ¼ � 100% (1) �
C.
k0
The experiment was conducted in the following process:
a. The polymer solution was prepared by polymer dry powder and
simulated injection water. The concentration of the polymer solution
Table 3 was 2000 mg/L.
Experimental data of polymer retention experiment. b. The porosity of the sand pack tube was measured using weight
Core Before flooding After flooding Residual Permeability method, and permeability measurement was conducted using Darcy’s
permeability k0 permeability kt resistance damage rate Law.
(10 3μm2) (10 3μm2) factor (%) c. At the injection rate of 1 mL/min, the sand pack tube was saturated
R1 161.36 1.954 82.40 98.79 with crude oil (72%) and formation water (28%), which was consistent
R2 291.35 7.482 38.94 97.43 with oil saturation in oil layer.
R3 395.03 29.371 13.45 92.56 d. The simulated injection water was injected into the sand pack tube
R4 1010.84 405.96 2.49 59.84
at the rate of 1 mL/min until the water cut was over 98%.
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F. Wang et al. Journal of Petroleum Science and Engineering 194 (2020) 107503
e. Then the polymer solution was injected into the sand pack tube at 2.9. Swelling experiment
the rate of 1 mL/min until pressure values kept stable.
f. The subsequent injection water was injected until pressure values The same-weight oilfield scale and oil-removing scale were respec
stabilized. tively added into the same-volume formation water. Then the mixtures
g. The pressure values at four pressure measuring points were real- were placed in the oven of 65 � C to soak for 12 h. The dissolution change
time recorded. And then the pressure drop values of four zones were and volume change of the two scale samples were observed.
calculated by pressure difference between adjacent pressure measuring
points.
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F. Wang et al. Journal of Petroleum Science and Engineering 194 (2020) 107503
3. Results and discussion with the interdependence and entanglement of various components.
3.1. Component analysis of the scale from polymer flooding 3.2. The sources of blockage
By drying the oilfield scale sample in the oven, it is found that there is Based on the component analysis of the oilfield scale, the genetic
a high content of water in the oilfield scale. By using Soxhlet extractor to mechanisms of various components and the interaction mechanisms
extract oil from the scale, it is proved that there is crude oil component among different components are discussed, and then the sources of
in the scale. blockage are obtained.
Through analyzing the infrared spectrum of the oilfield scale (Fig. 3
(a)), there is stretching vibration peak of 3421.4 cm 1 representing the 3.2.1. Scale source from injected fluid
–NH2 in primary amide, bending vibration peak of 1380.1 cm 1 repre With regard to polymer flooding, high molecular weight polymer is
senting the –CH2 group, stretching vibration peaks of 2940.8 cm 1 usually used to increase the viscosity of flooding system so as to improve
representing the –CH3 group, stretching vibration peaks of 1450.0 cm 1 the water/oil mobility ratio and finally enhance oil recovery. The par
representing the C–N in primary amide, stretching vibration peak of ticle size distribution of the oilfield polymer dry powder was studied and
1654.7 cm 1 representing the C– – O in primary amide, and stretching shown in Fig. 5 (a). It can be seen that polymer powder size distribution
vibration peak of 1050.3 cm 1 representing the C–N in quaternary is uneven and the proportion of polymer powder with particle size more
ammonium monomer. All of these peaks are consistent with the peaks in than 50 mesh is relatively high. Moreover, because of the space limita
the spectrum of polymer powder, which indicates polymer component is tion of offshore platform, the dissolution time of polymer powder in the
involved in the oilfield scale. dissolution tank is limited. With the limited dissolution time, small
Fig. 3 (b) shows the TGA curves of the oilfield scale and polymer particles can dissolve completely while large particles dissolve incom
powder. It is seen that the weight change of the scale can be divided into pletely. Therefore, there are a small quantity of incompletely dissolved
three stages during temperature rising process. In the first stage, the “fish eye” polymer particles (Fig. 5 (b)) carried by the completely dis
temperature is below 200 � C and a small amount of light oil volatilizes. solved polymer solution to the formation (Chen et al., 2011; Xu et al.,
In the second stage, the temperature is between 200 � C and 680 � C. 2005). Most of the “fish eye” particles are deposited in the near-injection
which is consistent with the degradation temperature of the polymer well zone, causing the blockage. A small portion of them are migrated to
powder. It can be deduced that the sharp decrease in scale sample deep zones of the oil layer.
weight is because of the polymer component degradation. In the third
stage, the sample weight remains unchanged while temperature con 3.2.2. Scale source from water incompatibility
tinues to rise. This is because the remaining inorganic components in the Through analyzing ionic composition and content of the injection
sample cannot degrade. water and the formation water, it is indicated that the injection water
According to the XRD spectra of the scale (Fig. 4), it mainly contains contains relatively high concentration of Ca2þ and Mg2þ while the for
tridymite (20.96), quartz and analcite (26.71), sodium feldspar and mation water contains high concentration of HCO3 and CO23 . With the
potassium feldspar (28.5), quick lime (40.00), and magnesia (42.5). The injection water and the formation water mixed under the reservoir
main components of tridymite, quartz, sodium feldspar, and potassium temperature, it can be observed that a large amount of white precipitate
feldspar are silica and silicate, which suggests the existence of rock appears in the mixtures. Fig. 6 is the XRD pattern analysis of the white
minerals. The main components of analcite, quick lime, and magnesia precipitate. There exist crystal forms of aragonite (26.33), calcite
are calcium carbonate and magnesium carbonate, which suggests the (29.57), dolomite (33.24), quick lime (39.57), and magnesia (43.04).
existence of carbonate components. The main components of these minerals are calcium carbonate and
The above results prove that components of the oilfield scale are magnesium carbonate, which suggests that incompatibility between
polymer, inorganic substances, water, and crude oil. In order to clarify injection water and formation water can contribute to the emergence of
the microscopic morphology of the scale, the scale morphology observed calcium carbonate and magnesium carbonate inorganic crystal
by SEM electron microscope is shown in Fig. 3 (c). It can be seen that the substances.
scale appears as composite aggregate formed by the entanglement of In order to further study the effect of polymer on the inorganic salt
polymer molecules in which a large number of inorganic particles are crystal, the polymer/injection water solution was also mixed with the
wrapped. The scale exhibits a large area of irregular surface. The result formation water under the reservoir temperature. Compared with mix
further illustrates that the oilfield scale is complex composite aggregate tures of injection water and formation water, there is more white pre
cipitate produced in the compounding solutions with polymer. So it can
be indicated that polymer molecules can combine with inorganic salt
crystal to form more precipitate. Besides, the inorganic salt crystal/
polymer composite scale simulation displacement experiment was car
ried out and its injection pressure curve is shown in Fig. 7 (a). After the
polymer/formation water solution is injected into the core, the injection
pressure increases significantly, which is mainly due to the displacement
effect of the high-viscosity polymer solution. When the injection water is
subsequently injected into the core, the injection pressure continues to
rise and fluctuate. The subsequent injection water can react with the
formation water in the core to generate inorganic salt crystal particles.
Afterwards, the polymer molecules can be adhered to these particles to
form the inorganic salt crystal/polymer scale, which severely blocks the
core pores and causes the injection pressure rising and fluctuating.
There has been much research on the interaction mechanism of
polymer molecules and inorganic salt crystal particles (Jordan et al.,
2005; Wang et al., 2006). It is widely believed that the inorganic salt
crystal produced by the water incompatibility can act as the crystal
nuclei. Due to the hydrogen bonding force, van der Waals force, and
Fig. 4. XRD pattern of the oilfield scale. electrostatic force, polymer molecules are easily adsorbed on the nuclei,
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F. Wang et al. Journal of Petroleum Science and Engineering 194 (2020) 107503
bridge blockage outside the narrow pore. Besides, with the flow of
flooding fluid, some precipitate can be carried and migrated to the
deeper zones of the oil layer.
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F. Wang et al. Journal of Petroleum Science and Engineering 194 (2020) 107503
blockage in the oil layer. Still, some scale is migrated forwards to the
production well direction.
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F. Wang et al. Journal of Petroleum Science and Engineering 194 (2020) 107503
3.3. Formation mechanism of blockage different. Because of the continual injection, the initial scale in near-
injection well zone is gradually migrated to the deep zones. In zone II,
Based on the analysis about the blockage sources, the consecutive there occurs massive deposition and bridge blockage of the migrated
formation mechanism of the blockage during polymer flooding can be scale. Meanwhile, the exfoliated fine particles can be blended in with the
concluded. After polymer solution is injected from the injection well, migrated scale to form the complex composite scale or directly interact
there are “fish eye” scale caused by imperfectly dissolved polymer with polymer molecules to form the flocculent scale. Due to the severe
powder and inorganic salt crystal/polymer scale caused by water in blockage caused by the migrated scale from zone I, the newly formed
compatibility and polymer enwrapping. The produced scale is deposited scale with fine particles cannot be migrated forwards effectively.
in the near-injection well zone or migrates to the deeper zones. During Therefore, with the polymer retention, the blockage in zone II is the
the migration, the exfoliated fine particles can be blended in with the most severe. In zone III, the blockage is caused by a small amount of
migrated scale, forming the composite scale with fine particles. Mean migrated scale from zone II, newly-generated fine particle/polymer
while, some exfoliated fine particles can directly interact with polymer flocculent scale, and polymer retention. In zone Ⅳ, there exists migrated
molecules to form the fine particle/polymer flocculent scale. These scale scale from zone III, newly-generated fine particle/polymer flocculent
with fine particles can form bridge blockage in the layer or migrate to scale, and slight polymer retention. Because there is major residual oil in
the production well direction. In the oil-bearing area near the produc this zone, the asphaltene from the crude oil can be further adsorbed on
tion well, the asphaltene from crude oil can be adsorbed and precipi the surface of the scale to form the oil-wrapped scale, which is more
tated on the scale surface to form an oil film, leading to the oil-wrapped firmly trapped in the layer and causes bridge blockage. In the subse
scale. The oil-wrapped scale is not easy to swell in the fluid and be quent water flooding stage, pressure drop values in all zones decrease
carried by the fluid. So it is firmly trapped in the layer and causes bridge slowly and then keep stable with being fluctuant. In this stage, the
blockage in the near-production well zone. In addition, polymer mole flexible blockage is gradually migrated and carried out from the pro
cules in the injected polymer solution can be adsorbed on the rock duction well. In the oil layer, there retains the stoutly-blocked and large-
surface and captured outside the narrow pore throat, diminishing the sized blockage. Overall, after multiple displacement stages, there exists
pore diameter and blocking the narrow throat. Especially, the inorganic blockage in all zones of the oil layer, with the most severe blockage in
particles formed by water incompatibility or fine particle exfoliation can the middle zone near the injection well (Fig. 12).
further aggravate the polymer capture and then cause more severe
blockage. Under the synergistic effect of scale formation and polymer 4. Conclusions
retention, with the oil layer adsorbed and captured by polymer, various
scale is deposited and bridge-blocked in the various zones of oil layer, (1) The component analysis indicates that the oilfield scale is
causing the blockage during the polymer flooding process. composed of polymer, inorganic substances, water, and crude oil.
Various components are interdependent and entangled with each
other in the scale.
3.4. Location distribution of blockage (2) After the polymer solution is injected into the formation, there
are two kinds of scale occurring in the near-injection well zone,
Based on the analysis of blockage formation mechanism during including “fish eye” scale and inorganic salt crystal/polymer
polymer flooding, the location distribution of blockage was further scale. With the scale migration and fine particle exfoliation, there
studied by physical simulation displacement experiment using the long forms the complex composite scale combined by migrated scale
sand pack tube. The simulated displacement process included three and fine particles as well as the newly-generated fine particle/
stages: water flooding stage, polymer flooding stage, and subsequent polymer flocculent scale. When the scale encounters with crude
water flooding stage. The pressure changing curves of various pressure oil, the asphaltene from crude oil can be adsorbed and precipi
measurement points and pressure drop changing curves of various zones tated on the scale surface, leading to the oil-wrapped composite
are shown in Fig. 11. According to the Darcy’s law, for the zone with scale. Besides, the injected polymer can be adsorbed and captured
higher pressure drop value, the permeability of this zone is lower and the in the oil layer, causing the decrease of the layer permeability.
seepage resistance is higher. So it can be indicated that the blockage of With decrease of oil layer permeability caused by polymer
the zone is more severe. Therefore, the location distribution of blockage retention, various scale is deposited and bridge-blocked in the oil
in the oil layer and its changes can be obtained by analyzing the pressure layer, causing the blockage during the polymer flooding process.
drop changing curves of various zones in various displacement stages. (3) After three displacement stages of water flooding, polymer
In the water flooding stage, the pressure drop in zone I is biggest and flooding, and subsequent water flooding, blockage is produced in
fluctuant, which suggests the inorganic scale caused by water in all zones of the oil layer. The blockage in the middle zone near the
compatibility is mainly concentrated in the near-injection well zone. In injection well is most severe.
the polymer flooding stage, the pressure drop in zone I increases and (4) The study will provide a theoretical basis for the subsequent
fluctuates significantly at first, indicating that a great deal of “fish eye” research on the blockage-removing fluid systems suitable for
scale and inorganic salt crystal/polymer scale is generated in the near- polymer flooding reservoirs.
injection well zone as well as the polymer retention. With the increase
of injection volume of the polymer solution, the pressure drop in zone I Declaration of competing interest
gradually turns down and the pressure drop values in zones II, III, and Ⅳ
gradually increase and fluctuate. The pressure drop in zone II rises to be The authors declare that they have no known competing financial
the biggest one while pressure drop values in other zones are not much interests or personal relationships that could have appeared to influence
the work reported in this paper.
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F. Wang et al. Journal of Petroleum Science and Engineering 194 (2020) 107503
Fig. 11. Pressure changing curves and pressure drop changing curves in physical simulation displacement experiment.
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