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Energy Procedia 63 (2014) 4638 4645

GHGT-12

The use of polymer-gel solutions for remediation of potential CO2

leakage from storage reservoirs
Amer Syeda, Benoit Pantinb, Sevket Durucana*, Anna Korrea and Ji- Quan Shia
a

Department of Earth Science and Engineering, Royal School of Mines, Imperial College London, London, SW7 2BP, UK.
b
Statoil ASA, Bergen, Norway.

Abstract
A polymer-gel based on Polyacylamide with Chromium as cross-linker was used and studied in order to ascertain its rheological
characteristics at various concentrations of polymer over a range of temperatures and salinities representative of the subsurface
conditions. Core flood experiments were carried out on a high permeability sandstone and fractured marble core samples to
investigate the flow characteristics of the polymer-gel in porous/fractured media. Laboratory core-floods revealed significant
reduction in permeability with different concentrations of polymer-gel in the injected water. Similar results were obtained for the
fractured core wherein a permeability reduction of 90% was noted, demonstrating the suitability of the system for possible
remediation of CO2 leakage through the caprock. Results from reservoir simulations supported the feasibility of polymer-gel
remediation at reservoir scale and identified the spatial extent of the leakage that can be remediated for various concentrations of
polymer-gel solutions.

Published
by Elsevier
Ltd. This
2014
2013The
TheAuthors.
Authors.
Published
by Elsevier
Ltd.is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/3.0/).
Selection and peer-review under responsibility of GHGT.
Peer-review under responsibility of the Organizing Committee of GHGT-12
Keywords: CO2 storage; leakage remediation; polymer-gel; permeability.

1. Introduction
Saline aquifers are seen as prospective industrial storage sites of anthropogenic CO2 due to their large storage
capacities. In comparison to other likely storage sites, such as the depleted hydrocarbon fields, knowledge on the
geological and petrophysical properties of saline aquifers is extremely limited. Hence a considerable degree of

Corresponding author. Tel.: +44-20-7594-7354; fax: +44-20-7594-7444.

E-mail address: s.durucan@imperial.ac.uk

1876-6102 2014 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/3.0/).
Peer-review under responsibility of the Organizing Committee of GHGT-12
doi:10.1016/j.egypro.2014.11.497

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Amer Syed et al. / Energy Procedia 63 (2014) 4638 4645

uncertainty in the conformance of CO2 flow in the subsurface in comparison to that estimated by
theoretical/numerical computations is expected. This unconformity may lead to undesired and unpredicted
preferential flow of CO2 into parts of the host reservoir or leakage into shallower formations. This paper investigates
the use of polymer-gel technology as one of the options to remediate non-conformal flow behaviour of CO2 in a
storage reservoir.
Crosslinked hydrolysed polymer-gel injection is used in petroleum industry to improve conformity of fluid flow
in the reservoir, remediate leakage around wells and also used in conjunction with enhanced oil recovery at various
temperature and pressure conditions [1, 2, 3, 4, 5] and to improve miscible CO2 floods [6, 7].
The structure of polymers is modified in time either by adding an additive, or just by interaction with the
environment (temperature, pressure or surrounding fluids). One important characteristic of polymers is swelling: it
adsorbs surrounding water and swell, thus occupying the pore volume available inside the rock and lowering its
permeability. Polymer solutions are composed of a carrier fluid (fresh water, brine, or gel) and plastic molecular
chains which are not attracted to each other due to the same surface potential charge. The low performance of
synthetic polymers in saline reservoirs is generally avoided by using a slug of fresh water as a front before the
polymer injection [8]. Therefore, when polymer solutions are used for CO2 leakage remediation, brine in the aquifer
must be carefully analysed to determine or even design a polymer solution to reduce the salinity effect on
performance. Hydrolysed polyacrylamide, in various proportions, is one of the widely used polymers within the
petroleum industry [9, 10]. Metal ions such as Cr(III) [11, 12, 13] and Aluminium [14] are widely used as a cross
linker.
2. Characterisation of the bulk polymer gel system
A polymer-gel is obtained by mixing a common polymer carrier fluid with a cross-linker to trigger a kinetic
reaction which bonds the molecular chains together. The unique property of a polymer-gel is its sudden increase in
viscosity, a phenomenon is referred to as gelation. The stage prior to gelation is referred to as the working time.
Gelation time is also defined as the time period when the elastic and viscous moduli of the gel become equal [15].
This time period depends on the characteristics such as chemistry, molecular weight and concentration of the
polymer, temperature, or cross-linker type.
Two types of Polyacrylamide polymers, SB-15 and AO-22, were sourced from SNF Folger, France. Both
polymers were delivered in an aqueous solution. During the laboratory experiments, Chromium (III) acetate was
used as the cross linker, as reported in a number of earlier studies in the literature [16]. The supplier recommended
composition of the crosslinker was 50,000ppm.
The first experimental step was to characterise the formation of gel. Different percentage mixtures of polymer and
chromium acetate were assessed during the experiments. Preliminary experiments carried out with increased
concentration of crosslinker indicated minimal or no impact on the gelation time. Hence for further work, the
solutions were prepared with increasing concentration of polymers: 2.1%, 4.1% and 6%. The cross linker
concentration in all cases was kept constant at 50,000ppm, in accordance with the suggestion of the supplier. Table 1
illustrates the properties of the prepared polymer gel solutions.
Table 1: Properties of polymers tested.
Polymer

SB-15

OA-22

Concentration in
solution [g/L]

Concentration of
polymer [%]

Po [mPa-S]

Uo [103 kg/m3]

150

2.1

0.98

1.02

300

4.1

1.00

1.02

440

6.0

1.01

1.02

100

2.1

1.05

1.02

200

4.1

1.08

1.02

300

6.0

1.12

1.02

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Fig. 1 presents the effect of polymer concentration on viscosity and working/gelation times for the two types of
polymers tested. The figure shows that an increase in polymer concentration accelerates the kinetics of the gel
reaction. For the lower concentrations of the polymer (2.1% or below), the polymer-gel system remains stable for at
least 20 hours, however, increase in the concentration of polymer results in the acceleration in the formation of gel
(Fig. 1a). From the perspective of subsurface operations, this working time could relate to the time during which the
polymer-gel can be injected into the reservoir before the gel solidifies and, with appropriate injection rate, the area
around the injection well can be covered.
10000%

100

Polymer SB-15: 2.1%,

Cr3+ : 50,000ppm, T: 20C

Polymer AO-22, Cr3+: 50,000ppm, T: 20C

Polymer SB-15: 1.4%,

Cr3+ : 50,000ppm, T: 20C

6000%

Working time (h)

Relative viscosity (/)

Polymer SB-15, Cr3+: 50,000ppm, T: 20C

Polymer AO-22: 2.1%,

Cr3+: 50,000ppm, T: 20C

8000%

Polymer AO-22: 4.1%,

Cr3+: 50,000ppm, T: 20C
Polymer AO-22: 6.0%,
Cr3+: 50,000ppm, T: 20C

4000%

Polymer SB-15: 4.1%,

Cr3+ : 50,000ppm, T: 20C

10

Polymer SB-15: 6.0%,

Cr3+ : 50,000ppm, T: 20C

2000%

0%
1

10

100

Time after cross-linker addition, hours

Percentage of polymer (%)

(a)

(b)

Fig. 1. (a) Viscosity evolution of polymers at different concentrations; (b) the effect of polymer concentration on working time of the two
polymers tested.

By applying the 200% threshold on the curves in Fig. 1a, the variation of the working time with increase in
polymer concentration is presented in Fig. 1b. At polymer concentration of 1.4%, the working time for polymer SB15 was found to be of the order of 100 hours ( 4 days), which decreases exponentially with increase in polymer
concentration. It can be inferred from Fig. 1 that the working time and the characteristics of reaction kinetics for
both polymers tested is almost identical. Based on this observation, it was decided to conduct further experiments
with AO-22 type of polymer only.
Measurements of polymer-gel system viscosities at constant temperatures (20, 40 and 80 oC) were carried out to
investigate the effect of reservoir temperature on gelation and working times (Figs. 2a and 2b). The experiments
indicate that the working time is significantly reduced at elevated temperatures. These results suggest that, for the
application of gel treatment in deep reservoirs, the concentration of the polymer must be low so as to attain desired
working time.
10000%

100

8000%

Polymer AO-22:
2.1%, Cr3+:
50,000ppm, T: 40C

6000%

Working time (h)

Relative viscosity (/)

Polymer AO-22: 2.1%, Cr3+:

50,000ppm

Polymer AO-22:
2.1%, Cr3+:
50,000ppm, T: 20C

Polymer AO-22:
2.1%, Cr3+:
50,000ppm, T: 80C

4000%

10

2000%

0%
0.1

10

Time after cross-linker addition, hours

(a)

100

0.1
0

20

40

60

Temperature, C

(b)

Fig. 2. Effect of temperature on viscosity evolution and working time of the AO22 polymer.

80

100

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3. Coreflood experiments using polymer gel solutions

Coreflood experiments were carried out using a high permeability sandstone and a synthetic fractured cap rock to
ascertain the applicability of the polymer-gel system in remediating the non-conformal flow of CO2 through the
reservoir and caprocks. Cylindrical samples of sandstone were cored out of a large block acquired from Doddington
quarry in Northumberland, England and a synthetic core was prepared from Carrara marble. Freshly drilled cores
were inserted into a Soxhlet [17] apparatus with continued circulation of toluene and methane for 24 hours in order
to remove any loose organic material from the porespace of the rocks. The rocks were then dried at 60 oC in an oven
for 24 hours followed by vacuum for 12 hours.
Porosity of the samples was measured using a pre calibrated Boyle's law pyconometer. Single phase CO2
permeability of the sandstone core samples was measured in a Hassler type core holder. Fig. 3 presents the
experimental set up used for polymer-gel core-floods and the Hassler type core holder which is used to apply a
constant confining stress of 3.5 MPa during the experiments. The upstream, downstream and confining pressures are
monitored by PDCR type pressure transducers supplied by GE/Druck UK. Two systems of flow lines on the
upstream end facilitate flow of fluid either at constant rate or pressure. Horizontal flow is ensured to minimise the
gravity effects. During the experiments, at any given instance, the supply is connected to one of these lines. The
pore fluids used in the experiments are polymer-gel system, gaseous carbon dioxide and brine. The brine is pumped
using a dual acting ISCO syringe pump of type 220D, supplied by Teledyne Inc., USA. The downstream end of the
cell is connected to an effluent collector. The main experimental set up, including the Hassler cell with pressure
transducers and effluent collector, is enclosed in a 170 litres Hereus type oven supplied by Thermo-Scientific GmbH
Germany, which was maintained at constant test temperature of 40oC. The core-flood experiments were carried out
following the procedure:
x
x
x

x
x

The prepared sample is first saturated with brine.

Gaseous CO2 is injected at constant flow rate to displace brine until the core is saturated with CO2 at
connate water saturation.
Pre-vacuumed ISCO syringe pump is used to inject prepared polymer-gel into the core at constant rate,
displacing CO2 in the process, until the core is saturated with polymer-gel at irreducible wetting phase and
residual CO2 saturation.
The upstream and downstream valves are shut and the polymer-gel in the porespace is left undisturbed for
24 hours to account for gelation time which is estimated from the polymer characterisation tests carried out.
CO2 is injected at constant pressure (~0.35 MPa) into the core sample to measure post-polymer injection
CO2 permeability and effectiveness of the polymer-gel system.
N2

Temperature
controller

12

14

Pump 1

13

Pump 2

9
5
11

CO2

3
4

10

1: precision pump
2: continuous flow pump
3: flow controlled line
4: constant pressure line
5: cleaning line
6: inlet pressure transducer
7: outlet pressure transducer
8: confinement pressure transducer
9: back pressure valve
10: collecting beaker
11: Hassler cell with core
12: pressure confinement line
13: pressure release line
14: oven at 40C

Fig. 3. Experimental setup for polymer floods in the laboratory.

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3.1. Effect of polymer concentration and reservoir salinity on permeability for CO2
The test conditions and the parameters considered for these experiments are presented in Table 2. For the first set
of experiments, the salinity of the brine was maintained constant at 3%. Three different mixes of the polymer-gel
solution were prepared and tested. Following brine saturation and drainage with injection of CO2, the polymer-gel
solution is injected into the sandstone core following the procedure outlined above. With the 2.1% polymer-gel
concentration, a substantial permeability reduction was observed: down from an initial permeability of 2,182 mD to
6.5 mD, representing a 99.7% reduction (Fig. 4a). Even greater reduction (over 99.99%) in permeability was
achieved with stronger gels, though the distance travelled from the injection point would decrease as the polymer
concentration increases, due to higher initial viscosity and reduced working time of the polymer solution.
Table 2. Experimental conditions used to assess the impact of polymer concentration and reservoir salinity on CO2 permeability.
Parameter

Polymer concentration
experiments

Reservoir salinity
experiments

3, 12, and 25

Salinity of brine [%]

Polymer concentration [aq. %]

2.1, 4.1 and 6.0

2.1

10-11

10-11

Capillary number [-]

Pore volume of CO2 injected [-]

Polymer-gel injection rate [m3/s]

0.0167

0.0167

4-5

4-5

50,000

50,000

Pore volume of polymer injected [-]

3

Crosslinker Cr+ [ppm]

Initial core permeability
Breakthrough permeability after gel treatment
Permeability reduction (%)
2180
2171

1500

2182

1928

2000

100%
99.7%

99.99%

Initial core permeability

Breakthrough permeability after gel treatment
Permeability reduction (%)

2500

99.99%

1000

500

Core permeability (mD)

Core permeability (mD)

2500

2147
1936

2000

1500

100%

99.7%

96.6%
89.1%

1000

500
235

6.5

0.0005

0.0015

Doddington 1,
Doddington 5,
Doddington 3,
Polymer AO-22: 2.1%, Polymer AO-22: 4.1%, Polymer AO-22: 6.0%,
Cr3+: 50,000ppm
Cr3+: 50,000ppm
Cr3+: 50,000ppm

(a)

50%

66

6.5
Doddington 1,
Brine: 3%NaCl

50%
Doddington 4,
Brine: 12%NaCl

Doddington 6,
Brine: 25%NaCl

(b)

Fig. 4. Effect of (a) polymer concentration and (b) reservoir salinity in reducing permeability for CO2 in Doddington sandstone samples due to
polymer-gel treatment.

In order to investigate the performance of polymer-gels in medium and large scale salinity environments two
further brine mixes of 12% and 25% were used in two new core-flood experiments (Table 2). Fig. 4b presents the
effect of salinity on the effectiveness of the polymer-gel solution in reducing permeability for CO2. General
observation from Fig. 4b indicates degradation of the polymer with increasing salt concentration. For example, an
increase in salinity from 3% to 12% led to a significant reduction in the effectiveness of the polymer solution, with
the destruction of the polymer chains. Nevertheless, nearly 90% reduction in permeability was achieved as shown in
Fig.4b. Further increase in the salinity to 25% had a similar impact, be it less pronounced, which calls for further
experiments. These results suggest that, for aquifers with high salinity, the use of polymer solutions may require a
well-planned and designed remediation strategy.

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3.2. Treatment of fractured rocks using polymer gel solutions

In order to investigate the performance of polymer-gel solutions to reduce the permeability of fractured rocks, a
similar approach to that reported in the literature [18] was followed. In order to ensure that the permeability is only
through the fracture and not through the rock matrix, a synthetic fractured core was prepared by cutting two Carrara
marble cores in the middle (Fig. 5a).
As the fracture has minimum or no residual wetting phase saturation, it was deemed appropriate to apply polymer
directly on the surface of fracture. Freshly prepared polymer-gel solution was applied to the two surfaces of the
fracture. The two pieces were then bonded with PTFE tape and the resulting sample inserted into the core holder and
left undisturbed at a constant confining pressure of 2 MPa to account for the gelation time. After gelation, CO2 was
injected from the upstream end of the core at constant pressure and flow rate. The same experiment was repeated
with different concentrations of polymer in solution (2.1%, 4.1% and 6.0%), similar to the experiments carried out
on the sandstone sample. The change in fracture permeability due to polymer-gel application is given in Fig. 5b.
10000

Initial permeability of fracture

Breakthrough permeability after gel treatment
Permeability reduction (%)
8100
8100

8100

Fracture permeability, mD

8000
100%
99.71%
92.44%

6000

97.65%

4000
50%

2000
613
0

24

Polymer AO-22: 2.1%,

Cr3+: 50,000ppm

(a)

190
0%

Polymer AO-22: 4.1%,

Cr3+: 50,000ppm

Polymer AO-22: 6.0%,

Cr3+: 50,000ppm

(b)

Fig. 5. (a) A synthetic fractured core prepared from Carrara marble; (b) the effect of polymer treatment on permeability for CO2 leakage through
fracture.

4. Numerical simulation of polymer injection

Reservoir simulations were carried out using a generic reservoir model in order to evaluate the suitability of
polymer-gel solutions in remediating the non-conformal flow of CO2 in a realistic CO2 storage scenario. The
reservoir model consisted of three zones: (a) Shallow aquifer: further divided into two layers (b) Caprock: further
divided into three layers, and (c) Host reservoir: further divided into six layers. The model was attributed with
uniform properties across the layers, with porosity and permeability values ranging between 0.1 0.2 and 0.0001
82 mD respectively, depending on the type of formation represented. At an assumed reference depth of 2,000 m and
a pressure of 20.3 MPa, the reservoir temperature and salinity were assigned as 93 oC and 3.5 (%vol) respectively.

Fig. 6. (a) Cross section of the reservoir model showing the injection well (2 vertical exaggeration); (b) location of leakage points (OP1, OP2
and OP3 ) on simulation grid (Layer shown is Layer number 3 of the caprock).

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In the near wellbore region, grid refinement was implemented at three levels as shown in Fig. 6b. The relative
permeability characteristics for the CO2 brine systems for reservoir modelling were adapted from the Viking
sandstone data reported by Bennion and Bachu [19].
Simulation of potential leakage of CO2 from the host reservoir into the shallow aquifer was assumed to be
through a fracture in the cap rock at one of the three locations identified as: (a) OP1: 200 m from the injection well
(b) OP2: 1,200 m from the injection well (c) OP3: 2,200 m from the injection well. Reservoir simulations have
indicated that it would take 2, 7 and 19 years for CO2 to be detected at leakage points OP1, OP2 and OP3 in the
shallow aquifer respectively.
As shown in Fig. 2 from the experimental results, the solution of 2.1% AO-22 polymer in water takes 20, 2.5 and
0.2 hours to form gel at 20, 40 and 80 oC. Extrapolating the experimental observations, it can be deduced that, at 93
o
C, the AO-22 polymer would form gel within 8 minutes of injection in comparison to 20 hours for similar reservoir
settings at 20oC. Under the given reservoir conditions of 20.3MPa pressure and 93 oC temperature, it was assumed
that only the polymer injection block would be saturated before the formation of solid gel, which would inhibit
further injection and transport of the polymer solution into the reservoir. And, assuming the polymer is injected
closer to the leak, the leaky grid block permeability was modified as per experimental observations, reflecting the
injection of polymer-gel.
Fig. 7a presents the amount of CO2 in dissolved, mobile and trapped phases in the shallow aquifer in case of
continuous leakage of CO2 from the host reservoir into shallow aquifer through OP1. As the leak was detected after
2 years in this case, the injection of CO2 was stopped and the permeability of leaky grid block at OP1 was modified
as 0.001mD, following experimental observations on permeability reduction for the fractured Carrara marble tested
at 20oC and 2.1% AO-22 solution in water. It was observed that, after remediation, the volume of CO2 leaked into
the shallow aquifer prior to the remediation progressively dissolves into the formation brine of the shallow aquifer
(Fig. 7b). A noteworthy observation is the absence of mobile CO2 within the shallow aquifer after remediation.
Similar observations were made for non-remediated and remediated leakages from OP2 and OP3.
Dissolved

1800

mobile

1600

trapped

200000

cumulative
150000

100000

50000

CO2 in shallow aquifer (tonnes)

CO2 in shallow aquifer (tonnes)

250000

Dissolved

1400
1200
1000
800
600
400
200

0
0

20
40
60
80
Time since leakage detection [years]

100

(a) No remediation. Leakage from OP1

20
40
60
80
Time since leakage detection [years]

100

(b) After polymer remediation (OP1)

Fig. 7. Phases of CO2 in shallow aquifer with and without remediation for leakage from OP1.

5. Conclusions
Laboratory experiments have shown that the gelation time for polyacrylamide based polymer gel systems
decreases with increase in polymer concentration. Furthermore, for identical combination of polyacrylamide and
Cr3+, the gelation time was found to decrease with increase in temperature. Laboratory core-flooding experiments on
high permeability sandstone cores saturated with 3% saline brine have shown reduction of more than 99% in gas
permeability at polymer concentrations of 2.1%, 4.1% and 6% in water. An increase in brine salinity generally leads
to the destruction of the polymer chains and a notable reduction in permeability. However, almost 90% reduction in
permeability was still achieved in higher salinity environments (12 to 25%). Polymer-gel treatment experiments on
fractured cores have shown that polymer-gel solutions would be effective in remediating leakage through fractures.

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4645

Results have shown around 93% to 99% permeability reduction depending on polymer concentration.
Laboratory measurements of gelation time and permeability reductions were used as input to a reservoir model to
assess the applicability of polymer gel remediation technique in the field. Results obtained from reservoir
simulations under scenarios simulated wherein CO2 is leaked from the host reservoir to a shallow aquifer through a
fracture in the caprock have indicated that injection of polymer-gel could potentially remediate the leak. In
summary, high molecular weight, anionic and hydrolised polymer chains such as poly acrylamide along with cross
linker such as Cr+3 can be used to remediate leakage of CO2 if the area of influence is carefully evaluated and the
injection process designed accordingly.
Acknowledgements
Research reported in this paper was conducted with funding from the European Commission FP7 project
CO2CARE, Grant Agreement No: 256625, and also co-financed by an industrial consortium consisting of Statoil,
Shell, TOTAL, RWE, Vattenfall, and Veolia. The Petrel and ECLIPSE 300 softwares used in this study is kindly
provided by Schlumberger. The polymers used were kindly supplied by SNF Folger, France.
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