SPE 110522
The Effect of Volume Changes Due to Mixing on Diffusion Coefficient Determination in
Heavy Oil and Hydrocarbon Solvent System
H. Luo, SPE, University of Calgary and TIPM Laboratory; D. Salama, SPE, Nexen Inc.; and S. Kryuchkov and A. Kantzas,
SPE, University of Calgary and TIPM Laboratory
Copyright 2007, Society of Petroleum Engineers
This paper was prepared for presentation at the 2007 SPE Annual Technical Conference and
Exhibition held in Anaheim, California, U.S.A., 1114 November 2007.
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Abstract
The diffusion coefficient is a key parameter to describe
promising solvent - based technologies for heavy oil and
bitumen recovery. In this work, an extended diffusion model
considering the volume changes on mixing was used to
calculate the mutual diffusion coefficients for the heavy oil -
hydrocarbon solvent system. The approach requires not only
concentration profiles, but also data on volume changes in the
process of mixing. The concentration profiles were obtained
from diffusion laboratory experiments in which X-ray
Computer Assisted Tomography (CAT) was used to measure
the density distributions at different times. In addition, the
volume changes data was obtained by performing heavy oil
and hydrocarbon solvent mixing experiments at different
content of solvent in heavy oil.
By comparing the diffusion coefficient versus
concentration curves based on the extended diffusion model
and on the usual diffusion model (1), it was concluded that the
volume changes due to mixing make significant differences to
the diffusion coefficient determination in heavy oil
hydrocarbon solvent system, and the mutual diffusion
coefficients are strong functions of concentration, which is
consistent with previous literature.
Introduction
With the introduction of the VAPEX process by Butler and
Mokrys (2) as an alternative heavy oil & bitumen recovery
technology, solvent - based processes seem to be more and
more promising because of their distinguished advantages,
such as: no heat loss, environmentally friendly, geologically
insensitive and so on. Since the injected solvent is less dense
and less viscous than the resident heavy oil & bitumen, the
solvent diffuses and/or disperses into the heavy oil, reducing
its viscosity. The solvent oil mixture then drains and is
recovered from the production well. Therefore mass transfer is
a crucial mechanism affecting the oil recovery rates in all
solvent - based processes including SAP (3) and warm VAPEX
(4)
. This makes it important to accurately evaluate the diffusion
coefficients of miscible solvents in heavy oil. However, mass
transfer between solvent and heavy oil and bitumen is a poorly
understood process. Currently the scarcity of reliable diffusion
coefficient values for such systems in literature is an obstacle
to the further development and application of solvent-based
processes.
Oballa and Butler (1), Das and Butler (5), Wen and
Kantzas (6), Salama and Kantzas (7) and Zhang and Shaw (8)
have obtained diffusion coefficients for heavy oil / bitumen -
solvent mixtures. They used measured concentration profiles
from laser or X-ray tomography, assuming the volume change
due to mixing to be zero. Both techniques measured local fluid
density, and then the density profiles were converted to
concentration profiles, assuming no volume changes on
mixing. However, data analysis of diffusion laboratory
experiments is particularly challenging. According to the
previous literature (7), the diffusion coefficients at early time of
diffusion are higher than the diffusion coefficients at later time
for the diffusion process of hydrocarbon solvents in heavy oil.
This phenomenon contradicts the generally acknowledged
theory that diffusion coefficients depend on concentration only
at the same conditions (same temperature, pressure and same
heavy oil solvent system). In addition, the diffusion
coefficient curves obtained by different researchers are
characteristic of different shapes. Therefore further
investigations are needed to understand better the mass
transfer phenomena in solvent - heavy oil and bitumen
systems. This paper focused on how the volume change on
mixing affects the diffusion coefficient values for the heavy
oil hydrocarbon solvent diffusion laboratory experiments.
The mathematical model
The inter-diffusion of two components forming a system in
which volume changes occur on mixing has been studied by
Prager (9). The rates at which the concentrations of the two
components CA and CB change at a point are given by
C A C A
= DA (vC A ) (1)
t x x x
C B C B
= DB (vC B ) (2)
t x x x
2 SPE 110522

DA and DB are the intrinsic diffusion coefficients for

component A and B, and v is the velocity of the mass-flow D = DAVBCB + DBVACA (10)
assumed to be in the x direction and dependent only on the x
coordinate and the time t. Equations (8) and (9) are the extended diffusion
Equations (1) and (2) are applicable to the systems in model used in this paper to describe solvent diffusion in heavy
the absence of thermal motion or forced diffusion, but in the oil considering the volume changes on mixing. The second
presence of volume changes on mixing. The diffusion process terms on the right-hand sides of equations (8) and (9) arise
discussed is based on the following assumptions: because of the volume changes on mixing, and they vanish
No chemical reaction occurs when such changes do not occur, in which case equations (8)
The system is contained in a static cell and (9) reduce to the usual diffusion equations.
There are volume changes on mixing If the initial distribution is such that
One dimensional diffusion in x direction
Constant temperature and pressure CA = 0, x < 0, t = 0,
There is a relationship between CA and CB at constant
temperature and pressure which is CA = C, x > 0, t = 0, (11)

VB CB + VA CA = 1 (3) then we can make the Boltzmann substitution if we suppose

CA to be a function of = x / (2t1/2) only. Thus equation (8)
where the VA and VB are the partial specific volumes of the two becomes
components A and B (10). Both VA and VB can vary with the
concentration at certain temperature and pressure conditions.
dCA d dCA d
2
D VB dCA
We also assume 2 = D CA d (12)
d d d d VB CA CA d
(C B / C A ) P .T = V A / VB (4)
with infinite boundary conditions
Using equations (3) and (4) in equation (2), and by doing
substitution, we find CA = 0, = -;
CA = C, = (13)
V C A V C A v V A C A
A = DB A C B + v (5)
VB t x VB x x VB x If the concentration distribution CA ( ) is known
from experiment, equation (12) can be solved for D to give:
And combining equation (5) with equation (1) yields
CA

CA CA xdCA
v C V C A 1 dx VB (14)
= VA DA A VB DB A (6) D= xdCA + CAVB dCA
x VB x
0
2
x x x 2t dCA 0 0 C V
A B
CA P,T

Integration by parts from - to x transforms equation
(6) into To satisfy the boundary conditions, the following
integral must be made equal to zero by adjusting the global
V C V C
C A
x
C
2 coordinate system for the bulk fluid motion.
+ B
D A + DB A A B A dx
v = V A ( D A DB )
x C A
VB C B C A x CA

....(7) C C xdC A
V B
xdC A + C V B dC A = 0 (15)
0

C A
2
where v and CA/ x have been assumed zero at x = - . 0 0 C AV B P ,T
Substituting equation (7) into equations (1) and (2), we have
Equation (14) was used here to calculate the mutual
diffusion coefficients based on the concentration distributions
CA CA D VB CA
x 2

= D CA dx (8) which were obtained in the solvent heavy oil diffusion

t x x x VBCA CA x experiments. The first term on the right-hand side of equation
(14) is the usual expression for calculating D from the
concentration profiles when there is no volume change on
CB CB D VB CA
x 2

x x x VBCA CA x
= D CB dx (9) mixing; the second term is a correction term because of
t volume changes on mixing.

where D is the mutual diffusion coefficient, and it is related to Principles of CAT scanning
DA and DB by X-ray CAT is an attractive tool for measuring the properties of
SPE 110522 3

reservoir fluids in a non-intrusive way (11). CAT scanning uses

an x-ray source that rotates around the sample to obtain one-
dimensional projections of x-ray attenuation at different angles
(12)
. As x-rays pass through the body to be scanned, they are 1200
absorbed or attenuated (weakened) at different levels creating y = 1.028x + 1034.923
1000
a matrix or profile of x-ray beams of different strength. This x- 2
R = 0.990

3
ray profile is registered by a series of detectors, thus creating 800

Density, kg/m
an image. From the one-dimensional projections, a cross
600
sectional slice through the sample is reconstructed in a
computer (13). 400
The basic quantity measured in each pixel of a CAT
200
image is the linear attenuation coefficient, , which is defined
from Beers law as (13) 0
-1200 -1000 -800 -600 -400 -200 0 200
CTn
I
= exp( h ) (16)
Io Figure 1: Liquid calibration curve for the GE9800 CT scanner

where,
Io The incident x-ray intensity 2500 y = 0.7477x + 907.3899
I The intensity remaining after the x- ray passes 2
R = 0.9851
through a thickness h 2000
X-ray attenuation factor in Hounsfield units (H.U)
3
Density, kg/m
1500
The scanner produces a CT number (11) array of each
image. CT attenuation data are normally presented in an 1000
internationally standardized scale called a Hounsfield unit,
which is defined by air at 1000H and water at 0H. These 500
units are calculated using the following equation (14):
0
1000 (i w ) -1500 -1000 -500 0 500 1000 1500 2000
CTn = (17)
CTn
w
Figure 2: Liquid/solid calibration curve for the GE9800 CT scanner
where,
CTn CT number for component i (H.U)
For illustration purposes, Figure 3 shows a CAT image
i X-ray attenuation of material i
of bulk oil sample topped with solvent at the beginning of the
w X-ray attenuation of water
experiment and after 14 days.
The x-ray attenuation factors depend on both bulk
density and atomic number as shown in eqation (18), hence
the produced CT numbers are proportional to the density of
the scanned sample.

= (a + bZ 3.8 / E 3.2 ) (18)

where,
Bulk density (kg/m)
Z Atomic number
a Energy-independent coefficient called Klein-
Nishina coefficient
b Constant
E Quantum of the X-ray energy (photon energy) Figure 3: CT scan of bulk oil topped with solvent at zero time and
after 14 days of starting the experiment
A series of calibration tests for liquid and solid
samples of known densities were performed in order to
correlate the CT numbers generated by the scanner to Using the correlation shown in Figure 1 and Figure 2,
densities. In Figure 1 and Figure 2 the calibration curves for the density of the scanned mixture was evaluated. It can be
liquid samples and liquid/solid samples are shown seen in Figure 3 that the solvent-bitumen interface becomes
respectively. Using these calibration curves, the densities of indistinct as time increases.
the scanned samples can be back calculated.
4 SPE 110522

Diffusion experiments 1. A Region of Interest (ROI) is cut where only the

The oil used in these experiments had a density of 0.978 g/cm3 mixture of oil/solvent is present, as shown in Figure 5.
at 25oC. The hydrocarbon solvent considered here is heptane. 2. The CTn of the ROI in the y direction is averaged; by
In Figure 4 the viscosities of the oil at different temperatures that obtaining CTn profiles of the mixture with height for
are plotted. As expected (15), the oil viscosity decreases each x value.
exponentially with temperature. 3. Using the density correlations for this specific scanner,
the CTn profiles were converted to density profiles. The
latter were then translated into concentration profiles
5
4.5 based on equations (19) - (22) which consider volume
log (Viscosity (mPa.s))

4 changes on mixing.
3.5
3
2.5 Vmn Con
2 Co = Con = (19)
1.5 V E + Vmn RV
1
0.5
n s RV s
0 Con = o m = o m (20)
15 20 25 30 35 40 45 50 55 60 65 70 75
o s o s
o
Temperature ( C)
n
V V + Vmn
E
RV = m = mn = (21)
Figure 4: Oil viscosities at different temperatures m Vm Vmn
Co C
Vmn = + 1 o s (22)
The experiments were conducted in sealed plastic and m o m
glass vials 125cm in volume (diameter: 4cm and height:
10cm). The diffusion process was monitored using the
where,
GE9800 CAT scanner. The procedure for this set of
Co Heavy oil mass concentration (g/cm3)
experiments is as follows:
1. The vial was filled with a predetermined amount of bulk Con Heavy oil mass concentration when no
heavy oil. volume change on mixing is assumed (g/cm3)
2. The vial was then scanned. Vmn Specific volume of mixture when no volume
3. Appropriate amount of a solvent was then added, and the change on mixing is assumed (g/cm3)
vial was properly sealed to prevent solvent weight losses. Vm Specific volume of mixture (g/cm3)
E
4. The vial was then scanned every 30 minutes for the first V Excess volumes of mixture (cm3/g)
three hours and then every three hours for at least seven o Density of heavy oil (g/cm3)
days. s Density of solvent (g/cm3)
m Density of mixture (g/cm3)
Image Processing m n
Density of mixture when no volume change
The following procedure was applied to analyze the scanned on mixing is assumed (g/cm3)
images: RV Relative volume

By simplifying equations (19) (22), a single

relationship formula (23) between Co and m can be obtained,
where VE is determined by doing heavy oil and solvent mixing
experiments. Because VE is the functions of Co itself, so this
approach needs iteration technique. The initial Co can be
calculated by equation (24). Figure (6) shows the calculated
concentration profiles in heavy oil - heptane diffusion
experiment.

o ( m s + V E m s )
Co = (23)
o s

s
Coi = o m (24)
o s

Figure 5: Bulk diffusion sample with the cut ROI shown

SPE 110522 5

From Figure 7, the excess volumes for the solvent

1.0 heavy oil system are negative and the volume change model is
Heavy oil concentration, volume fractio

Time: 1:05 hr reliable according to previous literature. Compared with

0.8
0.6
0.4
0.2
0.0
0.5
Figure 6: Oil concentration profiles in heavy oil - heptane
diffusion experiment
Volume changes on mixing
By doing heavy oil and solvent mixing experiments at
different mass ratios, the volume changes on mixing model for
heavy oil and solvent systems was obtained at room
temperature and atmospheric pressure. Here we assume that
heavy oil - solvent system is a binary mixture. In these mixing
experiments, the same heavy oil and solvent were used as
those in the diffusion experiments.
After mixing various amounts of heavy oil and
solvent completely, the density of the mixture was measured
with a Digital Density Meter, DMA 45. The accuracy of this
density instrument is 0.1mg/cm3. The measuring principle of
the instrument is based on the change of the natural frequency
of a hollow oscillator when filled with different liquids or
gases. Using a simple relationship shown in equation (25), the
total volume changes at different concentrations can be
calculated. Figure 7 shows the results of volume changes due
to mixing.
Time: 3:15 hr previously published experimental data (16) for binary
Time: 5:05 hr
hydrocarbon mixtures, we can see that the volume change
values are reasonable and the types of the excess volumes
versus concentration curves are similar. The difference is that
we use unit cm3/g for VE instead of cm3/mole, because the
heavy oil is actually a mixture of multi-components itself and
its pseudo-molecular mass is usually unknown. Then the
1.0 1.5 2.0 2.5 3.0 3.5 4.0 partial specific volumes VB in equation (14) can be obtained
Distance, cm easily based on equations (3) and (4).
Results and discussion
Diffusion experimental data at early time was chosen to
calculate the mutual diffusion coefficients, because of the
higher quality of the experimental data at early time without
large solvent vaporization loss.
The diffusion coefficients of the solvents in heavy oil
were calculated using the extended diffusion equations (14)
and concentration density relationship formula (23) which
consider the volume change on mixing. In order to compare
the results, the diffusion coefficients were also calculated
using the usual diffusion equation which only has the first
term on the right-hand side of equation (14) and concentration
density relationship formula (24) which assumes no volume
changes on mixing. Figures 8-9 show the comparison of
diffusion coefficient profiles based on different diffusion
models. It is obvious that considering the volume changes on
mixing, the diffusion coefficients change significantly. At
most concentration values the diffusion coefficients decrease.
24.00

m + m s mo m s Time: 1:05 hr- using the usual model

VE = o + / (m o + m s ) (25) 20.00
Time: 1:05 hr- using the extended model
m o s
16.00
where,
D, 10 cm /s
2

mo Mass of heavy oil (g) 12.00

-6

ms Mass of solvent (g)

8.00

Heavy oil concentration, mass fraction

0.00 0.20 0.40 0.60 0.80 1.00
4.00
0.00
0.00
-0.50 experimental data trend line
0.1 0.3 0.5 0.7 0.9
Volume changes, 10 cm /g
3

Heavy oil concentration, volume fraction

-2

-1.00

-1.50
Figure 8: Comparison of diffusion coefficient profiles using
different diffusion models at time 1:05 hr
-2.00

6 5 4 3 2
y = 118.73x - 396.87x + 515.75x - 331.54x + 116.68x - 22.804x + 0.0232
-2.50 2
R = 0.9732

-3.00

Figure 7: Volume changes on mixing for heavy oil heptane

system
6 SPE 110522

12.00 25.00

Time: 5:05 hr - using the usual model 20.00

10.00 Time: 1:05 hr

D, 10 cm / s
Time: 5:05 hr - using the extended model Time: 3:15 hr

2
15.00
8.00 Time: 5:05 hr
D, 10 cm /s

-6
2

10.00
-6

6.00
5.00
4.00
0.00
2.00 0.1 0.3 0.5 0.7 0.9
Heavy oil concentration, volume fraction
0.00
0.1 0.3 0.5 0.7 0.9 Figure 11: Diffusion coefficient profiles using the usual diffusion
Heavy oil concentration, volume fraction model

Figure 9: Comparison of diffusion coefficient profiles using

different diffusion models at time 5:05 hr
Figure 10 indicates the diffusion coefficient curves
using the extended diffusion model at different times and
Figure 11 shows the diffusion coefficient curves using the
usual diffusion model. We can see that the gap between
diffusion coefficient curves at different times is significantly
smaller when considering volume changes on mixing,
especially for the part with high heavy oil concentration. The
remaining differences could be due to the fact that heavy oil is
actually a mixture of substantially different components,
which have different diffusion coefficients.
Based on the results, the more important distinction is
that using the usual model, the far right end of diffusion
coefficient curves trend up with the heavy oil concentration
close to one; while using the extended diffusion model, this
phenomenon disappeared. It makes the diffusion coefficient
values more reasonable, since that the diffusion coefficients
should be smaller for the mixture with high content of heavy
oil in the hydrocarbon solvent heavy oil mixture.
We also can see that the mutual diffusion coefficient
is a strong function of concentration, considering the volume
changes on mixing, which is consistent with previous
literature.
25.00
20.00
D, 10 cm /s
Conclusions
1. The effect of volume changes due to mixing on the
diffusion coefficient determination is not negligible for
heavy oil - hydrocarbon solvent system.
2. Considering the volume changes on mixing, the diffusion
coefficients change significantly for the heavy oil -
hydrocarbon solvent system. At most concentration
values the diffusion coefficients decrease.
3. The phenomenon of the diffusion coefficients increasing
unconventionally with the heavy oil concentration close
to one disappeared using the extended diffusion model
which considers volume changes on mixing.
4. The gap between diffusion coefficients curves of
different times becomes significantly smaller when
considering volume changes on mixing, especially for
the part with high heavy oil concentration.
5. The mutual diffusion coefficient is a strong function of
concentration, even considering the volume changes on
mixing, which is consistent with previous literature.
6. The extended diffusion equations considering volume
changes on mixing can be used for the data analysis of
diffusion experiments to describe the diffusion process of
hydrocarbon solvents in heavy oil more accurately.
Acknowledgements
The authors wish to acknowledge the contributions of the staff
at the Tomographic Imaging and Porous Media Laboratory.
The authors are also grateful to ISEEE and the sponsoring
Time: 1:05 hr
Time: 3:15 hr
companies of the Canada Research Chair in Energy and
Imaging (Shell, Nexen, Canadian Natural, Devon Canada,

Time: 5:05 hr
2

15.00
Petro-Canada, E - T Energy, Suncor, Schlumberger, Laricina,
-6

10.00 Paramount, CMG foundation and Conoco Phillips) for

financial support.
5.00

0.00 Nomenclature
0.1 0.3 0.5 0.7 0.9 a= Energy-independent coefficient called Klein-
Heavy oil concentration, volume fraction Nishina coefficient
b= Constant
Figure 10: Diffusion coefficient profiles using extended diffusion CA = Concentrations of the component A (g/cm3)
model CB = Concentrations of the component B (g/cm3)
Co = Heavy oil mass concentration (g/cm3)
Co =
n Heavy oil mass concentration when no volume
change on mixing is assumed (g/cm3)
SPE 110522 7

CTn = CT number Oils with Hydrocarbon Solvents in the Presence of Sand,

D= Mutual diffusion coefficient (cm2/s) SPE/PS-CM/CHOA 97855, 2005 SPE International Thermal
DA = Intrinsic diffusion coefficients for component Operations and Heavy Oil Symposium, Calgary, AB Canada,
A (cm/s) Nov 1-3.
8. Zhang, X., Shaw, J.M.: Liquid-phase Mutual Diffusion
DB = Intrinsic diffusion coefficients for component Coefficients for Heavy Oil + Light Hydrocarbon Mixtures, Pet.
B (cm/s) Sci. Technol. (2007), 25, pg. 773.
h= Sample thickness 9. Prager, S.: Diffusion in Binary Systems, J. Chem. Phys. (Aug
I= The intensity remaining after the X-ray passes 1953), 21 (8), pg. 1344.
through a thickness h (kV) 10. Crank, J.: The Mathematics of Diffusion, 2nd edition, Clarendon
Io = The incident X-ray intensity (kV) Press, Oxford, (1975), pg. 234.
mo = Mass of heavy oil (g) 11. Kantzas, A.: Investigation of Physical Properties of Porous
ms = Mass of solvent (g) Rocks and Fluid Flow Phenomena in Porous Media Using
Computer Assisted Tomography, In Situ, (1990), 14(1), pg. 77.
ROI = Region of interest
12. Archie, G.E.: The Electrical Resistivity Log as an aid in
RV Relative volume Determining some Reservoir Characteristics, Pet. Trans. AIME,
t= Time (s) (1942), 146, pg. 54.
v= Velocity of the mass-flow (cm/s) 13. Vinegar, H.J.: X-ray CT and NMR Imaging of Rocks, J. Pet.
VA = Partial specific volumes of component A Tech. (March 1986), 38(3), pg. 257.
(cm3/g) 14. Cromwell, V., Kortum, D.J., Bradley, D.J. and Montana, C.:
VB = Partial specific volumes of component B The Use of a Medical Computer Tomography (CT) System to
(cm3/g) Observe Multiphase Flow in Porous Media, SPE Paper 13098,
VE = Excess volumes of mixture (cm3/g) 1984 SPE Annual Technical Conference and Exhibition,
Specific volume of mixture (g/cm3) Houston USA, September 16-19.
Vm
15. Bird, R.B., Stewart, W.E., Lightfoot, E.N.: Transport
Vmn = Specific volume of mixture when no volume Phenomena, 2nd edition, John Wiley & Sons Inc., New York
change on mixing is assumed (g/cm3) USA (2002), pg.22.
x= Space coordinate measured (cm) 16. Battino, R.: Volume Changes on Mixing for Binary Mixtures
Z= Atomic number of Liquids, Chem. Rev. (1971), 71 (1), pg. 5.
= X ray attenuation factor in Hounsfield units
(H.U)
i= X ray attenuation of material i
w = X ray attenuation of water
= Bulk density (g/cm)
o = Density of bitumen (g/cm)
m = Density of the oil and solvent mixture (g/cm).
mn = Density of mixture when no volume change on
mixing is assumed (g/cm3)
s = Density of solvent (g/cm)
= x / (2t1/2)

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