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Journal of Petroleum Science and Engineering


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A radiofrequency/microwave heating method for thermal heavy oil


recovery based on a novel tight-shell conceptual design
Matteo Bientinesi a,n, Luigi Petarca b, Alessandro Cerutti c, Mauro Bandinelli c,
Michela De Simoni d, Matteo Manotti d, Giuseppe Maddinelli d
a
Consorzio Polo Tecnologico Magona, via Magona, Cecina (LI) 57023, Italy
b
Dipartimento di Ingegneria civile e industriale, Università di Pisa, Largo Lucio Lazzarino, Pisa 56124, Italy
c
Ingegneria dei Sistemi, via Enrica Calabresi 24, Pisa 56121, Italy
d
Eni, Exploration and Production Division, via Emilia 1, San Donato Milanese (MI) 20097, Italy

art ic l e i nf o a b s t r a c t

Article history: The ongoing depletion of light oil resources and the increasing global energy demand is driving oil&gas
Received 10 October 2011 companies towards the exploitation of unconventional oil resources. In order to extract crude oil from
Received in revised form these resources, a sufficiently low oil viscosity must be achieved, for instance through temperature
8 February 2013
increase. Electromagnetic irradiation through downhole antennae can be a suitable method for in situ
Accepted 19 February 2013
heating of reservoirs. Potential problems for this technique are the extremely high temperatures that can
be reached at the well containing the radiating element and the strong dependence of temperature
Keywords: profiles on local variation of reservoir material properties. These problems can be solved to a large extent
enhanced oil recovery by inserting around the radiating well a tight shell made of a low loss dielectric material, and by selecting
thermal heavy oil recovery
the proper irradiation frequency.
electromagnetic heating
The experimental work described in this paper aims to verify the effectiveness of a similar structure
radiating antenna
oil sand during the electromagnetic heating of over 2000 kg of oil sand in a sandbox up to 200 1C, using a dipolar
modeling antenna. Oil sand was irradiated at 2.45 GHz frequency with variable power (1–2 kW). The temperature
in the oil sand mass and on the boundary were recorded throughout the test in several specific points, in
order to estimate temperature profiles along the distance from the antenna.
Experimental results confirmed that the presence of the low lossy material shell realized around the
antenna is extremely efficient in lowering the temperature in this critical zone and in better distributing
the irradiated energy in the oil sand mass.
& 2013 Published by Elsevier B.V.

1. Introduction drainage (SAGD) – are the main thermal methods currently


employed commercially. However, steam assisted oil recovery
The ongoing depletion of light oil resources and the increasing requires large amounts of fresh water, cannot be used for deep
global energy demand is driving oil&gas companies towards the or very shallow reservoirs, and its effectiveness depends on
exploitation of unconventional oil resources. These include viscous reservoir geological properties. The economical profitability or
crude oil reserves (heavy and extra-heavy oils), oil sand and oil even the technological feasibility of these methods can be greatly
shales. The International Energy Agency (IEA) estimates that there reduced in thin payzones, in low permeability formations, or in
are about 6 trillion barrels of such resources in place worldwide presence of a weak sealing cap rock (Clark, 2007).
(Clark, 2007). Electromagnetic (EM) irradiation, at radiofrequency (RF) or micro-
Due to high viscosity, heavy oils generally require enhanced oil waves (MW) frequencies, can be a sound alternative for in situ
recovery (EOR) techniques to be produced economically. Thermal heating of unconventional reserves. A RF/MW heating method, based
recovery methods, which introduce heat into the reservoir to on a downhole radiating antenna, is less affected by formation
reduce oil viscosity, are effective techniques to enhance heavy oil geology and is capable to distribute heat over a large reservoir
productivity. Steam injection processes – namely cyclic steam volume thanks to the propagation of electromagnetic energy through
stimulation (CSS), steam flooding (SF) and steam assisted gravity the medium. Other advantages are equipment compactness (suitable
for off-shore fields), high efficiency in the energy generation-
radiation process and the possibility to focus the energy on oil
n
Corresponding author. Tel.: +39 586 632142; fax: +39 586 635445.
bearing strata, reducing heat losses through the overburden.
E-mail addresses: matteo.bientinesi@polomagona.it (M. Bientinesi),
petarca@ing.unipi.it (L. Petarca), a.cerutti@ids-spa.it (A. Cerutti), Many industrial patents have been registered about this topic by
michela.de.simoni@eni.com (M. De Simoni). several companies in the last 60 years. Some examples are: Ritchey

0920-4105/$ - see front matter & 2013 Published by Elsevier B.V.


http://dx.doi.org/10.1016/j.petrol.2013.02.014

Please cite this article as: Bientinesi, M., et al., A radiofrequency/microwave heating method for thermal heavy oil recovery based on a
novel tight-shell conceptual design. J Petrol Sci Eng (2013), http://dx.doi.org/10.1016/j.petrol.2013.02.014i
2 M. Bientinesi et al. / Journal of Petroleum Science and Engineering ∎ (∎∎∎∎) ∎∎∎–∎∎∎

(1956), Haagensen (1965), Kasevich et al. (1979), Bridges et al. reservoir up to temperatures high enough to mobilize hydrocar-
(1979), Kiamanesh (1992), Kasevich (2008). Such patents describe bons at relatively long distances from the well and, in order to
set-ups based on the introduction of an electromagnetic power simplify the thermal resistance requirements for well completion
emitting apparatus in a well and differ from each other for materials, limiting near wellbore temperature. In another way, the
characteristics such as operating frequency, apparatus design and system aims to obtain temperature profiles versus the distance
well configuration. from the radiating element as uniform as possible.
In spite of the high number of patents, really few data were Fig. 1 shows one possible embodiment of the conceptual design
published demonstrating the applicability of this technique and of the new RF/MW method, in which a radiating antenna is
assessing its efficiency. In particular, three main lab-scale tests were coupled with a well-reservoir interface structure (tight shell)
presented: Sresty et al. (1986) verified the heating up to temperature whose scope is to limit temperature increase at the well. The
between 150 1C and 350 1C of a 300 kg Utah oil sand sample, system is composed by:
irradiated through a triplate line system; Kasevich et al. (1994)
irradiated a small sample of heavy oil through an antenna, while Hu  a production well (whose completion scheme is specially
et al. (1999) used two electrodes placed into a poly(methyl methacry- designed in order to host the RF/MW components and to allow
late) (PMMA) box to heat with radiofrequency (RF) a reconstructed oil EM irradiation);
sand sample. However, none of these authors show a temperature  a high power RF/MW energy applicator (composed by a surface
profile arising from electromagnetic irradiation, and little attention has unit with a high power RF/MW energy source, a downhole
been paid to the temperature reached in the vicinity of the wellbore transmission line and a bottom hole antenna);
during the irradiation process. This is one of the key issues of a RF/MW  a tight shell (a spherical or more likely cylindrical structure
reservoir heating technique. High reservoir heating rates require high interposed between oil well and reservoir, realized at the
EM power irradiation by the downhole antenna. This can turn out in antenna installation depth through drilling and completion
an extremely high EM field density located in the volume surrounding operations; the tight shell is made of a low loss dielectric
the radiating element. Reliable RF/MW heating processes must there- material and is impermeable to reservoir fluids).
fore take into account the EM energy distribution through the
reservoir and must be designed to achieve a volume heating as The same conceptual design can be applied also in configura-
uniform as possible. This is a key factor to prevent the exposure of tions where the RF/MW irradiation well is separated from the
well completion components to extreme temperatures, while irradiat- producer.
ing high EM power rates into the reservoir.
In order to meet the requirements addressed above, in the 2.2. Preliminary numerical simulations
present work a new RF/MW method, which combines a downhole
antenna with an interface structure realized between radiating In order to be feasible, the electromagnetic irradiation techni-
well and reservoir (called tight shell), is proposed. A theoretical and que must allow to heat large volumes of reservoir up to a
experimental study has been conducted to evaluate the potenti- temperature at which oil viscosity is low enough to be produced.
ality of the proposed solution and to design a RF/MW method Different heavy oils require different temperatures, varying from
capable to operate a high power, long term irradiation process, 70 1C to over 200 1C; in the preliminary study, we considered the
required to heat a considerable volume of reservoir. limit of 150 1C, over which the oil from the analyzed oil sand
In this paper we describe the novel tight shell conceptual samples has a viscosity lower than 100 mPa s. At the same time,
design, assessed by means of a simple numerical model and an maximum temperature at the radiating well must be kept at a
experimental test. The objectives are to assess the effectiveness of level tolerated by well completion materials; we considered 350 1C
the novel tight shell conceptual design and to study the different as the maximum temperature at the well for the present study.
phenomena taking place in a reservoir during electromagnetic Numerical simulations, performed varying a number of settings
irradiation and their effects on the application. such as reservoir material properties, irradiation frequency and
power, tight shell diameter, show that the operating system para-
meters have important effect on the thermal process, and the desired
2. Design of the system and preliminary modeling uniform heating can be achieved only with a proper system design.
In particular, the following general observation can be stated.
The new system design, described in what follows, was first
analyzed with preliminary numerical simulations.  Even changing reservoir material properties and system con-
In order to achieve short calculation times and a device as figuration, best irradiation frequencies turn out to be those in
flexible as possible, a simple numerical model was developed (as the 10–20 MHz range. Higher frequencies are as well capable to
described in Appendix A) assuming static conditions (no flow is heat deep into the reservoir, but temperature at wellbore
described) and spherical symmetry. This allows us to perform a results too high. This is shown clearly by the sensitivity analysis
wide spectrum of simulations in order to analyze: in Fig. 2, which describe the temperature reached at two
different distances from the antenna (0.15 m and 10 m) after
(1) the optimal operating frequencies to achieve homogeneous 1000 and 2000 days of irradiation at 200 kW for frequencies in
reservoir heating; the range 10–3000 MHz. Two temperatures are outlined in
(2) the impact of reservoir dielectric and thermal properties and Fig. 2: 150 1C is indicatively the minimal temperature to be
of operating conditions; reached at 10 m of distance from the antenna in order to
(3) the effectiveness of the tight shell solution and its design mobilize the oil, 350 1C is a limit for the temperature near the
parameters. wellbore in order to avoid structural problems. These limits can
change for different scenarios, in particular, several kinds of
heavy oil are mobile at much lower temperatures. Anyway, the
2.1. Novel tight shell system design fact that lower frequencies give a better energy distribution in
the reservoir can be generalized.
In order to optimize the electromagnetic heating process, a  The transient process of connate water evaporation in a volume
novel system was designed, with two main objectives: heating the surrounding the radiating antenna can remarkably reduce

Please cite this article as: Bientinesi, M., et al., A radiofrequency/microwave heating method for thermal heavy oil recovery based on a
novel tight-shell conceptual design. J Petrol Sci Eng (2013), http://dx.doi.org/10.1016/j.petrol.2013.02.014i
M. Bientinesi et al. / Journal of Petroleum Science and Engineering ∎ (∎∎∎∎) ∎∎∎–∎∎∎ 3

Fig. 1. Conceptual design of a production/radiating well with a spherical tight shell.

10000
r = 0.15 m; t = 200 day r = 10 m; t = 200 day
r = 0.15 m; t = 600 day r = 10 m; t = 600 day
r = 0.15 m; t = 1000 day r = 10 m; t = 1000 day

1000

350°C
Temperature [°C]

150°C
100
400

350

300

250
10
200

150

100
10 15 20 25 30 35 40 45 50

1
10 100 1000
Frequency [MHz]
Fig. 2. Frequency–temperature analysis for 200 kW irradiated power, 3 m radius tight-shell (tg(δ) ¼ 10−3). The diagram shows the temperatures reached at 10 m distance
from the radiating well (solid lines) and near the wellbore (circle spotted lines) for different irradiation times, as a function of the transmitted frequency (in the range
10–3000 MHz). In the window, the range 10–50 MHz is zoomed.

energy dissipation close to the well. This is due to the change in increase of salt water electrical conductivity (Hayashi, 2003),
dielectric properties of reservoir material, once the water has there is a fall of both quantities once the boiling point of
been removed, as shown as a way of example in Fig. 3 for an oil connate water (about 100 1C at atmospheric pressure for the
sand sample with an original water and oil content respectively analyzed sample) is reached and water is evacuated. This
of 4.2% and 10% by weight. Fig. 3 shows how, after a slight situation is representative of reservoirs in which both the oil
initial increase both of the real and imaginary part of the and the inorganic matrix are non-dispersive. Anyway, several
dielectric constant with increasing temperature, led by the oil sand, oil shale or heavy oil dry samples show higher values

Please cite this article as: Bientinesi, M., et al., A radiofrequency/microwave heating method for thermal heavy oil recovery based on a
novel tight-shell conceptual design. J Petrol Sci Eng (2013), http://dx.doi.org/10.1016/j.petrol.2013.02.014i
4 M. Bientinesi et al. / Journal of Petroleum Science and Engineering ∎ (∎∎∎∎) ∎∎∎–∎∎∎

20 60
T = 20°C
18 T = 50°C
T = 100°C 50
16
T = 125°C
14
40
12

ε''
10 30
ε'

8
20
6

4
10
2

0 0
10 100 1000 10 100 1000
Frequency [MHz] Frequency [MHz]

Fig. 3. Measurements of the real (left) and the imaginary (right) parts of dielectric permittivity of an oil sand sample with composition: 10% oil, 4.2% water, 85.8% quartz sand
by weight. The measurement is taken in the 10–1000 MHz range at 20 1C, 50 1C, 100 1C and 125 1C, according to the methodology described in Sarri et al. (2012).

500
800
450 700
600
400 500
400
350
300
Temperature [°C]

200
300
100
250 0
0 10 20 30 40 50

200
Tb = 160°C
150
ε'' (dry) = 0.1, 2000 d
100 ε'' (dry) = 0.1, 1000 d
ε'' (dry) = 0.01, 2000 d
50
ε'' (dry) = 0.01, 1000 d
0
0 5 10 15 20 25 30
Distance from antenna [m]
Fig. 4. Simulation results: comparison between thermal profiles obtained varying the dielectric properties of reservoir material after water evaporation, after 1000 and 2000
days of irradiation, without the use of the tight shell. Irradiation frequency is 10 MHz and emitted power is 200 kW. The water dried reservoir material has imaginary
dielectric constant ε″ ¼ 0.1 or 0.01. In the window, the full range 0–50 m is shown.

of imaginary dielectric constant, depending on oil composition nearby the antenna, but the extent of this reduction depends
(presence of polar compounds) or crystallographic composition on the reservoir pressure, which in turn determines the boiling
of the matrix (Friso et al., 1998; Kovalyova and Khaydar, 2004; temperature of connate water, and on the dielectric loss of the
Fuji et al., 1999; Saraev et al., 2005, Epov et al., 2009). Thus, we water dried reservoir material, which can vary significantly for
analyzed two different scenarios (see Fig. 4): for a non-lossy different reservoirs.
reservoir (ε″¼0.01), the temperature near the wellbore is  The heating process, realized without a tight shell interface, is
slightly above the boiling temperature of water in the reservoir then very sensitive to possible local variation of the reservoir
(about 160 1C for the analyzed scenario), since a volume of dielectric properties. In favorable conditions (low lossy solid
reservoir where water has been evaporated and electromag- matrix and heavy oil, and shallow reservoirs with depth lower
netic energy is poorly dissipated soon forms and increase its than 1000 m) water vaporization can be an effective “natural”
radius during the irradiation operation; for lossy reservoir (ε″¼ method to produce a uniform heating. Nevertheless the robust-
0.1), water evaporation is not sufficient to keep down the ness of a RF/MW method that relies only on connate water
temperature, since even in the dry volume dissipation takes vaporization appears to be dependent on dielectric properties
place, even if at a lower extent. We can then conclude that of materials, which, in real field operation, can be unknown or
water evaporation contribute to limit the temperature rise affected by reservoir heterogeneity.

Please cite this article as: Bientinesi, M., et al., A radiofrequency/microwave heating method for thermal heavy oil recovery based on a
novel tight-shell conceptual design. J Petrol Sci Eng (2013), http://dx.doi.org/10.1016/j.petrol.2013.02.014i
M. Bientinesi et al. / Journal of Petroleum Science and Engineering ∎ (∎∎∎∎) ∎∎∎–∎∎∎ 5

Simulation then focused on evaluating the effectiveness of the of the experimental set-up, as described in Appendix A, and was
new tight shell conceptual design in achieving a more uniform used to interpolate the data.
volume heating, limiting extreme temperatures nearby the
antenna, and to make the RF/MW method less dependent on
reservoir material properties. 3. Experimental methodology and material
In Fig. 5, we compare temperature profiles obtained with and
without the use of the tight shell (with 3 m radius) in the case of a The lab test was performed irradiating a sand box, properly
lossy reservoir (ε″ ¼0.1 for the dried material). The irradiation filled with oil sand, by an antenna and recording temperature data
frequency is 10 MHz and the emitted power 200 kW. It is evident along predefined sections. In what follows, the experimental set-
that a few meters radius shell would be sufficient to keep down up is described.
well temperatures, also in presence of a lossy reservoir medium
(ε″  0.1), in which case the temperature reduction caused by the
shell is dramatic. 3.1. Lab-scale experimental set-up
Several simulations were performed, varying the loss tangent
(tg(δ)) of the tight shell material between 10−4 and 10−3; in any The experiment was performed with a 2.45 GHz radiation. This
case, the tight shell turns out to be extremely successful in experimental choice, having a shorter wavelength and a smaller
lowering well temperature. Therefore, an effective tight shell penetration depth with respect to lower frequencies, allowed to
completion does not required a “very transparent” material (for reduce the oil sand amount needed, however providing reliable
instance, quartz sand and several proppants used in oil well experimental results.
applications, measured by Sarri et al. (2012), have tg(δ) 10−3).

2.3. Design of the experimental test

According to preliminary numerical results, the tight shell


turned out to be extremely effective in lowering the temperature
at the radiating well and in allowing to heat larger volumes of
reservoir. This conclusion led us to project and perform an
experimental test, with the major aim of evaluating the effective
decrease of the temperature near the wellbore arising from the
insertion of a low lossy material (tight shell) and the effect of
water evaporation on the development of temperature profiles.
Even though the optimal irradiation frequency was located
between 10 MHz and 20 MHz, an experimentation at these fre-
quencies would be hard to be performed with an antenna-like
emitting apparatus, if not directly on field, in a pilot well. As a
consequence, we chose to operate in the microwave range, at
2.45 GHz. The smaller wave length and penetration depth allowed
us to scale down the volume of interest, while still observing the
dielectric heating process and the temperature profiles developed
in the oil sand mass. The numerical model was adapted to the Fig. 6. Steel containment tank: the inner side of the walls are covered with radar-
radiation pattern of the experimental antenna and to the geometry absorbent material sheets.

500
1000
450 No tight shell, 1000 d
800 No tight shell, 2000 d
400 3 m tight shell, 1000 d
600
3 m tight shell, 2000 d
350 400
Temperature (°C)

300 200

250 0
0 10 20 30 40 50
200
Tb= 160°C
150

100

50
r=3m
0
0 5 10 15 20 25 30
Distance from antenna (r)
Fig. 5. Simulation results: comparison between thermal profiles obtained without the tight shell or using a 3 m radius spherical shell (constituted by a material with tg(δ)¼
10−3) after 1000 and 2000 days of irradiation. Irradiation frequency is 10 MHz and emitted power is 200 kW. The water dried reservoir material has imaginary dielectric
constant ε″ ¼0.1. In the window, the full range 0–50 m is shown.

Please cite this article as: Bientinesi, M., et al., A radiofrequency/microwave heating method for thermal heavy oil recovery based on a
novel tight-shell conceptual design. J Petrol Sci Eng (2013), http://dx.doi.org/10.1016/j.petrol.2013.02.014i
6 M. Bientinesi et al. / Journal of Petroleum Science and Engineering ∎ (∎∎∎∎) ∎∎∎–∎∎∎

The mass of oil sand used in the experiment has a base


dimension 1.25  1.25 m and a height of 0.75 m. The choice of
the dimensions depended on preliminary simulations results and
on the antenna design; the latter has in fact a dipole-like, non-
spherical radiation pattern which extends more in the horizontal
direction than in the vertical one. To properly fill the space, the
samples were shaped in cubic blocks pressed into a mold of proper
shape. In order to press the blocks, oil sand material was heated up
to 70/80 1C, turning it malleable; each produced block weighed
between 28.5 kg and 32 kg, resulting in a void grade of 2–10%, with
an average value of 3%; 73 blocks were used, for a total amount of
over 2200 kg of oil sand material. The oil sand assembly was
confined by a steel containment tank (Fig. 6).
On the base of the tank, a 100 mm thick layer of quartz sand
was poured. On this layer, oil sand blocks were then assembled,
leaving between each block a 10 mm thick gap, filled again with
quartz sand. A vacant position was left in the center for the
insertion of the antenna (Fig. 7) and a cylindrical hole was realized,
in which the antenna was placed (Fig. 8). In the cylindrical hole, Fig. 8. Realization of the cylindrical hole for the introduction of the antenna and
optical fiber positioning.
two concentric polytetrafluoroethylene (PTFE) tubes, closed at the
bottom, were installed. Outside the outer tube, a low lossy quartz
sand was poured, realizing a cylindrical shell. The gap between Several fiber optic temperature sensors were inserted in
outer and inner tube was filled with the silicone oil Rhodorsil Oil selected oil sand blocks, in the quartz sand shell and in the silicone
47 V20 (Bluestar silicones). The inner tube contained a rigid oil between the two PTFE tubes. In addition, several K-type
coaxial line, terminating with the antenna (Fig. 9). thermocouples were used to monitor the temperature of the outer
The internal face and the base of the containment tank were surface of the steel walls.
covered with sheets of radar-absorbent material (RAM, Eccosorb The position of the various sensors is illustrated in Fig. 12,
SF2.5), glued to the metal with a room temperature vulcanizing where a section of the experimental set-up, at the height of the
(RTV) silicone adhesive. The RAM absorbs all the electromagnetic center of the antenna, is depicted. Fiber optic sensors (FO##,
radiation reaching the tank walls, converting it into thermal where ## is a number) and thermocouples (TC##) recorded the
energy and avoiding reflection of microwaves by the steel walls. temperature continuously. TCx (x being a letter) indicates the
Fig. 10 shows the schematic of the experimental set-up. The thermocouples located in the gap between different oil sand
microwaves are generated by a water cooled magnetron with a blocks, which periodically measured the temperature at different
maximum output of 2 kW, fed by a switching power generator, depths, after temporarily stopping the irradiation.
commanded via PC. Downstream the magnetron, an isolator The position of the fiber optic sensors was defined in order to
avoids the reflected microwaves to come back to the magnetron; record the temperature profiles versus the distance from the
the reflected power is measured through a linear power sensor. antenna, at the height of the antenna itself, where the radiating
Microwaves travel through a waveguide from the control room power is at its maximum. The fiber optic sensors provided the
to the experiment room. Through an adapter, microwaves are temperature profile in the main direction A and allowed to
transferred into a rigid coaxial line, terminating in the antenna confirm the individuated trend on two other directions (B and C,
situated in the exact center of the oil sand mass (Fig. 11). as defined in Fig. 12).
The experiment room is thoroughly ventilated in order to In order to obtain a good contact between the probes and the
remove any gas possibly exhaled by the heated oil sand. However oil sand material, once a sensor had been inserted in the pre-
operators were not allowed into the room throughout the drilled block, oil (originating from the same oil sand samples) was
experiment. poured (at a temperature of 80 1C) in the hole in order to assure
the immobilization of the probe and the thermal equilibrium.
The thermocouples attached to the outer side of the tank walls
were used to qualitatively evaluate the thermal energy dissipated
by natural convection towards the surrounding environment.
Table 1 defines the position of each temperature probe,
assuming (Fig. 12) an xyz coordinate system with the origin at
the center of the antenna.

3.2. Antenna design and testing

The project of the antenna was developed through four stages:


requirements analysis, antenna type selection, antenna simulation
and individuation of mechanical devices for impedance adjust-
ment and return loss minimization.
Requirements analysis lead to the individuation of the follow-
ing specifications:

 geometrical specifications (maximum diameter 60 mm);


 operating frequency 2.45 GHz;
Fig. 7. Assembling of the oil sand cubic blocks. Noteworthy, the bottom layer is
complete while the central layer, as well as the not shown top layer, has a vacant  return loss lower than 10 dB;
position in the center for the introduction of the antenna.  radiation diagram optimized for power radial distribution.

Please cite this article as: Bientinesi, M., et al., A radiofrequency/microwave heating method for thermal heavy oil recovery based on a
novel tight-shell conceptual design. J Petrol Sci Eng (2013), http://dx.doi.org/10.1016/j.petrol.2013.02.014i
M. Bientinesi et al. / Journal of Petroleum Science and Engineering ∎ (∎∎∎∎) ∎∎∎–∎∎∎ 7

The antenna was designed through simulations with a modeling  a rigid coaxial line with the inner conductor opportunely longer
tool developed by IDS (Ingegneria dei Sistemi), considering the than the external conductor;
environment in which the antenna is inserted for the experiment  several circular elements terminating the inner conductor,
(PTFE tubes, silicone oil, low lossy sand shell, oil sand). The which are useful for impedance adjustment;
projected antenna (Fig. 13) is constituted by:  a mobile choke, which is used to decrease return currents on
the outer conductor and to adjust antenna impedance.

Once the antenna was realized, the return loss was measured
using a Network Analyzer (Agilents PNA-X-N5242A) in several
configurations, and specifically in air, sand, wet sand, as well as in
the experimental set-up before and after filling the tank with oil
sand. The return loss at 2.45 GHz, in the definitive set-up, turned
out to be −29 dB. The antenna is moreover extremely adaptable to
different parameters of the surrounding environment.

3.3. Reservoir and tight shell materials

Two different bulk materials were used to fill the sand box in
the experimentation, namely:

 oil sand samples, furnished by Eni;


 low lossy quartz sand.

Fig. 9. Insertion of the PTFE tubes and of the radiating element in the low lossy
sand shell. Fig. 11. Experimental set-up.

Fig. 10. Schematic of the experimental set-up and identification of the main equipment.

Please cite this article as: Bientinesi, M., et al., A radiofrequency/microwave heating method for thermal heavy oil recovery based on a
novel tight-shell conceptual design. J Petrol Sci Eng (2013), http://dx.doi.org/10.1016/j.petrol.2013.02.014i
8 M. Bientinesi et al. / Journal of Petroleum Science and Engineering ∎ (∎∎∎∎) ∎∎∎–∎∎∎

Fig. 12. Position of fiber optic sensors and of thermocouples for temperature
measurements.

Table 1
Position of temperature sensors during oil sand electromagnetic heating experi-
mental testing. The coordinate system used has origin in the center of the antenna,
and is depicted in Fig. 8.

Fig. 13. MW radiating antenna.


FO## x y z TC## x y z TCx x y
[mm] [mm] [mm] [mm] [mm] [mm] [mm] [mm]

FO1 200 0 0 TC2 0 −650 0 TCa 390 0 Temperature data from fiber optic sensors and thermocouples
FO2 320 0 0 TC3 0 650 0 TCb −390 0 were recorded with a frequency of 60 records per hour. Periodi-
FO3 460 0 0 TC4 −650 0 0 TCe 0 390
cally, power was briefly switched off in order to measure the
FO4 0 −260 0 TC5 650 −319 0 TCf 0 −390
FO5 580 0 0 TC7 650 0 0 TCt 85 0 temperature at different depths.
FO6 40 0 0 TC9 650 319 0 In Table 4, the journal of the experiment is reported. Note-
FO7 60 0 0 TC14 650 0 250 worthy, radiating power was first set at 1000 W and then
FO8 −520 0 0 TC16 650 0 −250 increased to 1500 W and 2000 W once a quasi-stationary tem-
FO9 −260 0 0
FO10 120 0 0
perature profile was achieved. Finally, in order to further increase
the temperature in the oil sand, the outer side of the metallic walls
and the top surface were covered with 5 cm thick rockwool
These materials were characterized through a series of techni- insulating panels. The experiment lasted over 13 days.
ques described in Sarri et al. (2012). The results of interest are
reported in Table 2 for oil sand and in Table 3 for quartz sand.
About the dielectric properties of oil sand samples, they remain 4. Results and discussion
practically stable with increasing temperature as long as connate
water evaporation is limited while, after water evaporation, 4.1. Experimental results
imaginary permittivity decrease significantly (Table 2).
The type of quartz sand used was selected for its particularly Fig. 14 shows temperature data from all the sensors placed in
low imaginary permittivity, which makes it a really low lossy the A direction (see Fig. 12), for the entire duration of the
material, thus particularly suitable for the tight shell simulation experiment. In particular, seven fiber optic sensors (FO6, placed
(though the shell is not actually tight in this specific case). in the silicone oil between the two concentric PTFE tubes, FO7 and
FO10, inserted in the quartz sand shell, and FO1, FO2, FO3, FO5, in
3.4. Electromagnetic heating experiment the oil sand) and one thermocouple (TC7) are considered. These
data have to be analyzed taking into account the actions occurred
A long term experiment was conducted in order to: during the experiment, as reported in Table 4.
Figs. 15 and 16 report the time evolution of the temperature
(1) evaluate the time evolution of temperature profiles at different profile along the x coordinate (see Fig. 12), during the first part of
radiating power levels; the experiment and after the thermal insulation of the set-up
(2) compare experimental data with the numerical model devel- respectively.
oped and described in Appendix A; Fig. 17 shows the time evolution of the temperature profile
(3) evaluate the degree of mobilization of the bitumen in the along the z coordinate in the point TCa (see Fig. 8), at a distance of
temperature range 150–200 1C. 390 mm from the antenna.

Please cite this article as: Bientinesi, M., et al., A radiofrequency/microwave heating method for thermal heavy oil recovery based on a
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M. Bientinesi et al. / Journal of Petroleum Science and Engineering ∎ (∎∎∎∎) ∎∎∎–∎∎∎ 9

Some main observations can be made based on these results: (Fig. 15); this arises from the evaporation of the small amount
of connate water present and the subsequent decrease of oil
 oil sand temperature increases monotonically during electro- sand loss tangent. The water evaporation clearly contributes to
magnetic irradiation due to the dielectric heating phenomenon
(Figs. 14–17); 220
 notwithstanding the higher electromagnetic field present as a 200
consequence of the smaller distance from the antenna, the
180
temperature of the quartz sand shell (FO7 and FO10 sensors in
160
Fig. 14 and x o200 mm in Figs. 15 and 16) is always lower than

Temperature [°C]
the maximum temperature achieved in the oil sand material 140

(FO1 sensor in Fig. 14), thus confirming the efficiency of the 120
shell design in decreasing the temperature around the well and 100 FO6, 40 mm
the antenna; FO7, 60 mm


80 FO10, 120 mm
once the temperature of the oil sand material overcomes
60 FO1, 200 mm
100 1C, a sensible decrease in the heating rate can be observed FO2, 320 mm
40 FO3, 460 mm
Wall
insulation FO5, 580 mm
20
Table 2 TC7, 650 mm

Average properties of oil sand material used in the experimentation. 0


0 24 48 72 96 120 144 168 192 216 240 264 288 312 336

Property Value Time [h]

Fig. 14. Temperature measured by the sensors placed along direction A (see Fig. 12)
Sand void grade 40%
for the entire duration of the experiment. In the legend, the distance of each probe
Water content 0.25 wt%
from the antenna is reported.
Oil content 13 wt%
Dielectric constant ε′ 3.8
(@ 2.45 GHz, 25 1C) ε″ 0.1 140
Dielectric constant ε′ 2.5 0h
5h
(@ 2.45 GHz, 4100 1C) ε″ 0.01 120 10 h
Density 2100 kg/m3
15 h
Specific heat (@ 25 1C) 930 J/kg K
Temperature [°C]

20 h
100
Thermal conductivity (@ 25 1C) 0.93 W/mK 25 h
30 h
80 35 h
40 h

60
Table 3
Properties of quartz sand used in the experimentation. 40

Property Value
20
Dielectric constant ε′ 2.9
(@ 2.45 GHz, 25 1C) ε″ 0.001 0
Bulk density 1620 kg/m3
0 50 100 150 200 250 300 350 400 450 500 550 600 650
Void grade 39.1% x [mm]
Specific heat (@ 25 1C) 800 J/kg K
Thermal conductivity (@ 25 1C) 0.24 W/mK Fig. 15. Temperature profiles in the direction A (see Fig. 12) versus the distance
from the antenna, before set-up thermal insulation.

Table 4
Journal of the experiment.

Time Action

0 Magnetron switched on, power 1000 W. Start recording temperature data


17 h 15 min Magnetron switched off, measure with thermocouples (MTC1)
17 h 22 min Magnetron switched on, power 1000 W
28 h 46 min Magnetron switched off, measure with thermocouples (MTC2)
28 h 56 min Magnetron switched on, power 1500 W
36 h 16 min Magnetron switched off, measure with thermocouples (MTC3)
36 h 30 min Magnetron switched on, power 2000 W
61 h 42 min Magnetron switched off, measure with thermocouples (MTC4)
61 h 54 min Magnetron switched on, power 2000 W
68 h 59 min Magnetron switched off
69 h 02 min Magnetron switched on, power 2000 W
86 h 33 min Magnetron switched off
86 h 36 min Magnetron switched on, power 2000 W
165 h 51 min Magnetron switched off, measure with thermocouples (MTC5)
166 h 02 min Magnetron switched on, power 2000 W
183 h 21 min Magnetron switched off, steel wall and top surface covered with fiberglass insulation
183 h 56 min Magnetron switched on, power 2000 W
205 h 55 min Magnetron switched off
205 h 57 min Magnetron switched on, power 2000 W
232 h 29 min Magnetron switched off
232 h 38 min Magnetron switched on, power 2000 W
326 h 06 min Magnetron switched off, measure with thermocouples (MTC6), insulation removed

Please cite this article as: Bientinesi, M., et al., A radiofrequency/microwave heating method for thermal heavy oil recovery based on a
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10 M. Bientinesi et al. / Journal of Petroleum Science and Engineering ∎ (∎∎∎∎) ∎∎∎–∎∎∎

limit temperature rising near the well and favors the penetra- removed from the walls through natural convection of the
tion of electromagnetic energy; surrounding air. This leads to avoid heat accumulation into the
 the silicone oil temperature (FO6 in Fig. 14) increases initially up oil sand thus providing boundary conditions that can be
to 70 1C; once this temperature is reached, convective motions roughly representative of a larger oil sand mass (obviously this
establish, favoring the dissipation of heat towards the environ- holds as long as the set-up is not thermally insulated);
ment through the upper surface of the fluid; this heat dissipated  the measured vertical temperature profiles show a maximum
is the cause of the qualitative difference between the curves for for z ¼0 (Fig. 17), i.e. on the horizontal plane intersecting the
the tight shell scenario in Fig. 5, where the temperature center of the antenna, decreasing quasi-symmetrically upwards
maximum is always at the antenna, and the curves in Fig. 15; (zo 0) and downwards (z 40), in agreement with the predicted
 the temperature of the external metallic walls (curve TC7 in pattern of the antenna;
Fig. 14) is determined by two concurrent phenomena: on one  the final phase of the experiment, after the insulation (see
side, the RAM sheets absorb practically all the residual electro- Fig. 16), is used exclusively in order to increase the temperature
magnetic energy reaching the borders, on the other side, heat is over to 100 1C in the whole mass of oil sand, allowing to evaluate
the possible mobilization of the oil at higher temperatures. Once
the set-up was dismounted, oil sand blocks were visually
220 analyzed and several points, where the oil partially had drained,
200 were detected (Fig. 18). It is clear that for this specific oil sand
180 sample gravity drainage is not sufficient, even at high tempera-
160 ture, to obtain a significant oil mobilization.
Temperature [°C]

140
120 4.2. Comparison with the numerical model
100
80 40 h
The numerical model was adapted, as described in Appendix A,
180 h to the geometry and radiation pattern of the experimental set-up,
60
200 h in order to compare simulation results with experimental results.
40 230 h
In the model, material properties are time-independent, thus
20 260 h
320 h the model is adequate to experimental data description only for
0 temperature below the boiling point of water (100 1C). Above this
0 50 100 150 200 250 300 350 400 450 500 550 600 650
temperature, water vaporizes and escapes from the oil sand mass,
x [mm]
dielectric permittivity decreases and electromagnetic energy dis-
Fig. 16. Temperature profiles in the direction A (see Fig. 12) versus the distance sipation decreases as well.
from the antenna, after set-up thermal insulation. In Figs. 19 and 20, experimental temperature profiles in the r
and z directions are compared with simulation results. Noteworthy
the agreement is excellent as long as the temperature of 100 1C is
200 not overcome; once the water contained in the oil sand is
17 h
180 29 h evaporated, the model is no longer valid and thus the prediction
36 h of temperature profiles becomes largely inaccurate.
160 62 h
166 h
140 326 h
Temperature [°C]

120 5. Conclusion

100
This paper presents a novel design for the downhole electro-
80 magnetic heating of oil sand/heavy oil reservoir, including a tight
60 shell made of low lossy material inserted in the surrounding of the
well containing the radiating antenna. Preliminary numerical
40
simulation performed with a simplified model showed that the
20
presence of a tight shell could help to reach uniform heating of
0 large volumes of reservoir avoiding the risk of high temperatures
-350 -300 -250 -200 -150 -100 -50 0 50 100 150 200 250 300 350
at the wellbore, and making the recovery method much less
z [mm] sensitive to local dielectric properties of the reservoir materials.
Fig. 17. Temperature profiles along the vertical coordinate in the point TCa (at a An experimental test was set up to confirm these claims.
distance of 390 mm from the antenna along the direction A, see Fig. 12). Experimental results showed that electromagnetic irradiation is

Fig. 18. Oil draining from oil sand at the end of the test.

Please cite this article as: Bientinesi, M., et al., A radiofrequency/microwave heating method for thermal heavy oil recovery based on a
novel tight-shell conceptual design. J Petrol Sci Eng (2013), http://dx.doi.org/10.1016/j.petrol.2013.02.014i
M. Bientinesi et al. / Journal of Petroleum Science and Engineering ∎ (∎∎∎∎) ∎∎∎–∎∎∎ 11

180 Appendix A
1h
3h
160
5h The numerical model describes the coupled electromagnetic
10 h
140
15 h and thermal problem related to RF/MW irradiation of a heavy oil
20 h reservoir through an antenna installed inside a wellbore, at an oil
Temperature [°C]

120
25 h
bearing level. Fluid flow due to production is not considered.
28 h
100 The problem is governed by the equation of thermal energy
80 conservation
∂T
60 ρeff C eff −∇  ðK eff ∇TÞ ¼ q ðA1Þ
∂t
40
where ρeffCeff and Keff are respectively the effective heat capacity
20 and the effective thermal conductivity of the reservoir material,
0 and q is the heat source term which accounts for the energy
0 100 200 300 400 500 600 released per unit time and unit volume by the electromagnetic
x [mm] field into the reservoir.
In order to calculate the q term, the following equation, which
Fig. 19. Comparison between experimental (symbols) temperature profile along x
and simulation results (continuum lines). governs the attenuation of the irradiated energy flux (Von Hippel,
1966), is first solved

180 dPðrÞ
¼ −2αPðrÞ ðA2Þ
17 h 15 min
dr
160 28 h 46 min
36 h 13 min where P is the electromagnetic wave power per unit solid angle
140
62 h 00 min irradiated by the antenna, r is the coordinate along the wave
Temperature [°C]

120 propagation direction, and α is the electromagnetic wave attenua-


100
tion coefficient.
The attenuation coefficient α is a function of the wave
80
frequency and of the complex dielectric permittivity of the
60 material
40 vffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
0sffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi 1
u  
u
20 n 2πf uε′mix @ ε″mix 2 A
α ¼ αðf ; εmix Þ ¼ t 1þ −1 ðA3Þ
c 2 ε″mix
0
-350 -300 -250 -200 -150 -100 -50 0 50 100 150 200 250 300 350
z [mm] where f is the wave frequency, c is the speed of light in vacuum,
ε′mix and ε″mix are the real and imaginary part of the complex
Fig. 20. Comparison between experimental (symbols) temperature profile along z
in the point TCa (r¼ 390 mm, see Fig. 12) and simulation results (continuum lines). dielectric permittivity of the reservoir medium, which is a mixture
of different components (namely solid matrix, oil and water).
Hence, α is not actually constant but varies with time and with the
capable of heating oil sand, even above the boiling temperature of spatial coordinate, as a consequence of material compositional
connate water. The low lossy material shell realized around the changes (water vaporization).
antenna turned out to be efficient in lowering the temperature in Once provided the solution of the EM power field P(r), the heat
this critical zone, as demonstrated by the fact that the maximum source term can be calculated applying the following equations
temperature is reached outside the shell. ! !
In a real oil well, from a technical point of view a 3 m radius q¼−∇  F ðA4Þ
tight shell is hardly feasible with current technologies but future
studies will be performed in order to asses if less stringent PðrÞ
FðrÞ ¼ ðA5Þ
temperature limits and the effect of convective cooling due to r2
fluids flow could lead to significant shell radius reduction. where F(r) is the electromagnetic energy flux (i.e. the energy
It was moreover shown that water vaporization has a signifi- carried by the electromagnetic wave crossing the unit area per
cant impact on temperature profiles and contributes to limit the unit time).
temperature rise near the wellbore region and to better distribute In order to study the effect on the reservoir heating process, the
the irradiated energy in the reservoir. model was configured to take into account water vaporization.
Current ongoing activities are aiming to develop a more A strong assumption we make is that the produced steam can
realistic reservoir model that includes a 3D geometry, the con- escape the reservoir and does not cause a pressure increase. This
vective term in the thermal equation, as well as oil and water flow, assumption is hardly realistic, but it significantly simplify the
in order to assess the effective benefits of the designed system in model. The reservoir is ideally divided in three zones, with
terms of oil recovery and productivity index improvement. different dielectric and thermal properties:

 water saturation zone (with T oTboil): dielectric and thermal


properties of the reservoir are those of the rock-heavy oil–
Acknowledgements water system (dielectric properties are assumed equal to the
values measured at 20 1C and shown in Fig. 3);
Eni, e&p division, is gratefully acknowledged for funding this  boiling layer zone (T  Tboil): transition phase for a little interval
research activity and providing reservoir materials for the experi- around Tboil; the reservoir thermal capacity is calculated so as
mental activities. to include the water evaporation latent heat;

Please cite this article as: Bientinesi, M., et al., A radiofrequency/microwave heating method for thermal heavy oil recovery based on a
novel tight-shell conceptual design. J Petrol Sci Eng (2013), http://dx.doi.org/10.1016/j.petrol.2013.02.014i
12 M. Bientinesi et al. / Journal of Petroleum Science and Engineering ∎ (∎∎∎∎) ∎∎∎–∎∎∎

Table A1
Setting for numerical simulation for the comparison with experimental results.

Parameter Value Observation

Transmitted power, P0 1000 W (for


0o t o29 h)
Well radius, r0 47.5 mm External PTFE tube radius
Shell radius, rshell 125 mm Low lossy quartz sand shell radius
Tank radius, rcont 650 mm Minimum distance between the antenna and the lateral walls of containment tank
Initial temperature, T0 16 1C Measured
Temperature of the outer walls (boundary T0+0.714 t [min] From the interpolation of data measured with thermocouples on the external walls
condition), Text
Temperature of the upper and bottom walls T0 Equal to the temperature of the room
(boundary conditions), Text
Boundary condition at the well dT/dr¼0.5 K/mm This condition arises from the average value of heat dissipated through the silicone oil
throughout the trial
Sand shell permittivity, εshell 2.9−i0.001 Measured (Sarri et al., 2012)
Oil sand samples permittivity, εOS 3.8−i0.1 Measured (Sarri et al., 2012)
Shell sand density, ρshell 1620 kg/m3 Measured
Shell sand specific heat, Cshell 900 J/kg/K Measured (average value in the range 20–200 1C)
Shell sand thermal conductivity, Kshell 0.1 W/m/K Measured (average value in the range 20–200 1C)
Oil sand samples density, ρOS 2000 kg/m3 Calculated from the measured values of density of the components bitumen, connate water,
sand, and from the measured composition
Oil sand samples specific heat, COS 1020 J/kg K Measured (average value in the range 20–200 1C)
Oil sand samples thermal conductivity, KOS 0.8 W/m/K Measured (average value in the range 20–200 1C)

 dried zone (for T 4Tboil): dielectric and thermal properties of In order to compare simulation results with experimental
the reservoir are those of the rock-heavy oil system, from which results, the model was adapted to the geometry and to the
water has been removed (dielectric properties are assumed radiation pattern of the experimental set-up. Two major modifica-
equal to the values measured over 100 1C and shown in Fig. 3). tions were made:

These three zones evolve with time, determining the material  a 2D axisymmetric geometry was used in substitution of the
properties to be used in Eq. (A1) and Eq. (A2) at a certain time for a spherical geometry;
given value of the spatial coordinate.  material properties dependence on temperature was neglected
The described physical model is implemented using Comsol for simplicity.
Multiphysics, in a 1D spherical geometry. Initial and boundary
conditions are: The choice of a 2D geometry is determined by the fact that the
radiation pattern of the experimental antenna is not isotropic but
 thermal equation: dipole-like, so focused in the horizontal plane and symmetric with
 uniform temperature (25 1C) for t¼ 0 through the entire respect to the vertical axis, with a 3 dB gain in the direction of
domain; maximum irradiation. In order to simulate the distribution of
 adiabatic boundary condition at the well, imposed by the energy in the material, a 2D axisymmetric geometry was adopted
symmetry of the problem; and an analytical expression was used for the approximate
 constant temperature at the outer boundary, equal to the initial calculation of the radiation diagram:
temperature (this condition is justified by the fact that the 4
f pattern ðθÞ ¼ 2  sin ðθÞ ðA6Þ
considered domain is much larger compared with the heating
radius; where θ is the polar angle.
 electromagnetic wave attenuation equation (since this is a first Considering material properties independent of temperature, it
order, stationary equation, it requires a single boundary was possible to write the analytical solution of the heat source
condition): term in the thermal balance
 boundary condition at the well, where P0 is the total power 8 2αshell P 0 f pattern ðθÞ
< r 0 o r ≤r shell ⇒qðr; θÞ ¼ exp½−2αshell ðr−r 0 Þ
irradiated by the antenna. 4πr 2
: r shell o r o r cont ⇒qðr; θÞ ¼ 2αOS P 0 f pattern ðθÞ
4πr 2
exp½−2αshell ðr shell −r 0 Þexp½−2αOS ðr−r shell Þ
The setting of reservoir material parameters in the model is ðA7Þ
based on dielectric and physical characterization, carried out on oil
sand samples. Detailed description of the experimental laboratory where P0 is the transmitted power, αshell and αOS are the attenua-
set-up and of the methods for the RF/MW dielectric characteriza- tion coefficient in the shell and in the oil sand respectively, r0 is the
tion and for the measure of thermal properties of reservoir well radius, rshell is the radius of the shell and rcont is the minimum
materials is provided by Sarri et al. (2012). distance of the containment tank wall from the axis of the
Other relevant settings used in the preliminary numerical antenna.
simulations are: Attenuation coefficients, αshell and αOS, were calculated from
experimental data on the dielectric permittivity of the two
 reservoir average depth 80 m; materials at the frequency of 2.45 GHz
 vffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
1ffi
reservoir pressure 6 bar; u 0sffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
 2
u
 boiling temperature of connate water 160 1C; 2πf u ε′
t @ 1þ
ε″
αðf ; εn Þ ¼ −1A ðA8Þ
 sand porosity 25%; c 2 ε′
 initial water saturation 23%;
 initial oil saturation 77%; Since material properties are considered independent of tem-
 latent heat of vaporization of water 2080 kJ/kg. perature, the model is adequate as long as these properties do not

Please cite this article as: Bientinesi, M., et al., A radiofrequency/microwave heating method for thermal heavy oil recovery based on a
novel tight-shell conceptual design. J Petrol Sci Eng (2013), http://dx.doi.org/10.1016/j.petrol.2013.02.014i
M. Bientinesi et al. / Journal of Petroleum Science and Engineering ∎ (∎∎∎∎) ∎∎∎–∎∎∎ 13

differ significantly from their values at room temperature. This is Hayashi, M., 2003. Temperature-electrical conductivity relation of water for
what happens experimentally once the connate water in oil sand environmental monitoring and geophysical data inversion. Environ. Monit.
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both the real and the imaginary part of the oil sands permittivity. electromagnetic heating. Energy Source 21, 63–73.
Thus, we expect the model to be accurate in interpolating experi- Kasevich, R.S., Kolker, M., Dwyer, A.S., 1979. In situ radio frequency selective heating
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Kiamanesh, A.I., 1992. In situ tuned microwave oil extraction process. US Patent
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novel tight-shell conceptual design. J Petrol Sci Eng (2013), http://dx.doi.org/10.1016/j.petrol.2013.02.014i

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