Journal of Petroleum Science and Engineering 74 (2010) 3140

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Journal of Petroleum Science and Engineering

j o u r n a l h o m e p a g e : w w w. e l s ev i e r. c o m / l o c a t e / p e t r o l

Experimental and visual analysis of diffusive mass transfer between matrix and
fracture under static conditions
Can Ulas Hatiboglu 1, Tayfun Babadagli
University of Alberta, Department of Civil and Environmental Engineering, School of Mining and Petroleum, 3-112 Markin CNRL-NREF, Edmonton, AB, Canada T6G 2W2

a r t i c l e i n f o a b s t r a c t

Article history: This study investigates miscible interaction between oil saturated porous rock and solvent lled fractures
Received 25 June 2008 driven by diffusion and natural convection. This type of mass transfer interaction is commonly encountered
Accepted 9 August 2010 during enhanced oil recovery applications, groundwater contamination, underground waste disposal, and
greenhouse (mainly CO2) sequestration. The rst part of the study focuses on the visual analysis of the transfer
Keywords:
of a hydrocarbon solvent into oil saturated rock to clarify the physics of the interaction process. The second
oil recovery
groundwater contamination
part consists of a series of core experiments to compare the oil recovery performances of the mass transfer
CO2 sequestration process.
naturally fractured reservoirs 5 cm diameter and 5 cm long cylindrical Berea sandstone samples were coated with epoxy to create co- and
miscible displacement counter-current type interactions. Mineral oil and kerosene were used as oleic phases and n-heptane was
diffusion used as a solvent. Aged samples were also included in the experiments. The effects of interaction type (co- or
natural convection counter-current) and direction (horizontal, vertical, and inclined), aging, gravity, and oil viscosity on the rate
mass transfer of oil recovery by diffusion and ultimate oil recovery were claried. The core experiments were compared to
effective diffusion coefcient
the equivalent 2-D visualization experiments conducted on 5 5 0.03 cm sand pack models to account for
the dynamics of the process.
Finally, a quantitative analysis was performed and the effective diffusion coefcients obtained from the slope
of the loglog plot of the recovery-time plots were correlated to the rock and uid properties.
2010 Elsevier B.V. All rights reserved.

1. Introduction
For an efcient recovery of oil from naturally fractured reservoirs,
the interaction between the matrix and fracture needs to be
accelerated using different enhanced oil recovery techniques. Like-
wise, using injected gas during greenhouse gas sequestration or waste
disposal applications, the injected material should be transferred into
the rock matrix for permanent storage.
The conventional practice in oil reservoirs is to ood the reservoir
with water, where the recovery is obtained by spontaneous imbibition if
the reservoir is naturally fractured. This method is efcient if the matrix
is water-wet and enough of the immiscible wetting phase exists in the
fracture. This type of recovery enhancement may not be adequate if the
matrix is oil wet or the displaced phase is high in viscosity. In these cases,
more expensive thermal applications need to be considered. Due to an
increasing demand for oil and the requirements for CO2 sequestration,
miscible displacement (solvent injection) has become an alternative
option.
It is well known that a substantial amount of oil (residual oil)
might be left in the matrix even in strongly water-wet systems
Corresponding author.
E-mail address: tayfun@ualberta.ca (T. Babadagli).
1
Now with Shell Canada.
(Mattax and Kyte, 1962; Bourbiaux and Kalaydjian, 1988; Ma, et al.,
1995; Zhang, et al., 1996; Kantzas et al., 1997; Schembre et al., 1998;
Babadagli, 2001; Zhou et al., 2002; Hatiboglu and Babadagli, 2007,
2008a). Tertiary recovery of this remaining oil using heat or solvent
could be effective but characteristically inefcient, as the process is
uncontrollable due to the high permeability fracture network that
controls the ow direction of the injected uid (Da Silva and Belery,
1989; Morel et al., 1993; Zakirov et al., 1991; Le Romancer et al., 1994;
Lenormand et al., 1998; Stubos and Poulou, 1999; LaBolle et al., 2000;
Rangel-German and Kovscek, 2002; Polak et al., 2003; Hatiboglu and
Babadagli, 2008a).
If the injected solvent is the hydrocarbon type, its retrieval is a
critical issue in naturally fractured reservoirs and the combined
application of thermal and miscible injection could be a solution for
this problem (Al-Bahlani and Babadagli, 2009a,b). Also, in the case of
CO2 injection in naturally fractured reservoirs, permanent storage of
CO2 in the matrix part should be considered to make the enhanced oil
recovery application efcient and feasible (Trivedi and Babadagli,
2008a,b, 2009a,b).
In light of the above listed efforts, we designed a set of experiments
to analyze the physics of solvent diffusion into porous media under
static conditions to mimic miscible interaction between the matrix
and fracture in naturally fractured reservoirs. Core experiments
were conducted using different rock samples. The core experiments

0920-4105/$ see front matter 2010 Elsevier B.V. All rights reserved.
doi:10.1016/j.petrol.2010.08.004
32 C.U. Hatiboglu, T. Babadagli / Journal of Petroleum Science and Engineering 74 (2010) 3140
revealed that interaction by diffusion needs to be analyzed for
different oil viscosities, interaction type, and gravity. Hence, we
conducted equivalent 2-D visualization experiments and extensive
analyses of the observations combined with the core experiments.
We chose sand pack models for visualization to clarify interesting
but inexplicable observations on the recovery curves obtained from
the core experiments. The reason behind this choice was the extreme
cost and effort needed for the 3-D visualization of the experiments on
cores of that size. 2-D visual and 3-D core models are not identical
in terms of porosity and permeability but they represent exact
characteristics of matrix boundary conditions, orientation of interac-
tion, and viscosities.
2. Experimental procedure
Oil saturated core samples were exposed to the solvent by
immersing the samples into solvent lled containers to mimic miscible
ooding in fractured reservoirs (hydrocarbon or CO2 injection into oil
reservoirs) (Fig. 1). The process was represented by oil recovery
against time plots. The second group of experiments consists of
visualization experiments that were carried out as a means of support
to corresponding core experiments (Fig. 2). To have a clear under-
standing of the dynamics of the process, 2-D glass-bead packed
transparent models were used. Cores were chosen with the same aspect
ratio as the visual glass-bead models. Variables for both core and
visualization experiments are listed as:
(1) Interaction type: Co- and counter-current manner,
(2) Oil type: Kerosene and mineral oil,
(3) Orientation: Horizontal, vertical, and inclined,
(4) Effect of aging time.
2.1. 2-D visualization experiments
2-D sand pack models were prepared using two inch thick
transparent acrylic sheets. The gap between the acrylic sheets was
kept as 0.3 mm and was lled with 0.1 mm diameter glass beads. The
dimensions of the models are 5 5 0.03 cm. Utmost attention was
paid to pack the glass beads densely to assure a homogeneous
distribution. A lter paper was used to prevent glass-bead loss and to
provide better contact of the diffusing phase with the displaced uid
(a)
Scales
Continuous
weight
monitoring
Hanging core samples
Fig. 1. (a) Experimental set-up for solvent diffusion experiments on the cores, (b) interaction process for the counter-current case (open side downwards).
(oil) at the side of the model from which the diffusing phase entered.
The models were sealed with epoxy only on the two sides, and both
sides and the top for the co- and counter-current experiments,
respectively. A compatible epoxy sealant was selected to not react
with the pentane. Fig. 2 shows an outlook of the model and the
experimental set-up. Table 1 provides the properties of the uids used
in the experiments. In all experiments, each model was used for only
one experiment to avoid any wettability change due to the cleaning
process. Oil samples used (kerosene and mineral oil) are standard
ones available in the market and contain no heavy polar components
to avoid any signicant change on rock surface properties. Details of
the experiments are given in Table 2.
The models saturated 100% with either mineral oil or kerosene
under a vacuum were put into contact with pentane either
horizontally, vertically, or inclined at 10. In both the co- and
counter-current cases, the bottom edge was immersed into the
pentane. In the co-current case, the top edge was open to the
atmosphere, whereas for the counter-current case it was sealed with
an epoxy. Note that the experiments conducted in this study were at
zero initial water saturation which is not representative of reservoir
conditions. Also, the oils used in this study were either mineral oil or
kerosene, which are not representative of reservoir conditions. They
were chosen because of simplicity and obtaining clear images to
analyze, which was not practically possible with any crude oil.
The horizontal case had its limitations: a fan-cooled high-intensity
halogen light source had to be used to supply enough illumination
since the light has to be powerful enough to be transmitted through
both the model and the reservoir of the diffusing uid. In the
horizontal case, the model was tilted slightly upwards so as to not
have any pentane contact with the upper portion of the model. The
bottom part was fully immersed into the pentane. Fig. 2 illustrates the
experimental set-up.
In the vertical cases, a weaker light source was good enough to
obtain good quality images, as the light had to be transmitted only
through the 2-D model. Time lapse photography using a 6.3
megapixel camera served to visualize the experiments. Images
transferred to a computer were processed using open-source software
(ImageJ), which has multi-image stack handling capability (Rasband,
19972005).
Since it was difcult to construct a sturdy and homogeneous 2-D
sand pack model with all sides open to ow case, it was decided to use
(b)
Epoxy
coating
Oil
saturated
sample
Oil Solvent
mixed
with solvent
 C.U. Hatiboglu, T. Babadagli / Journal of Petroleum Science and Engineering 74 (2010) 3140
(a)
Computer
Model
Light source
Camera
MicroPump
Fig. 2. Experimental set-up for 2-D visualization experiments: (a) vertical, and (b) horizontal sample positioning.
a medium porosity lter paper as the porous medium for this type of
conguration and one experiment was conducted on this type of
model before starting the sand pack experiment with sealed edges.
The model was saturated with kerosene and immersed into the
pentane in a horizontal orientation for those preliminary experiments
(Fig. 3). The process was observed to be random, generating diffusion
limited aggregation (DLA) type patterns. The oil recovery occurred
from the same side as the solvent phase entered the model.
In addition to the all side open model (Fig. 3), a counter-current
model with only one edge open to interaction was also tested using a
lter paper as the porous medium (Fig. 4). When another boundary
condition (three-side-sealed) that results in fully counter-current
interaction was applied, a different frontal progress was observed.
Although ngering was observed in the early stages of the process (in
the rst 3 min), the displacement front turned out to be much
smoother than in the previous case. The process started from the sides
where there is less resistance to ow. The central portion began to
contribute much later.
2.2. Core experiments
The recovery curves were obtained for Berea sandstone samples
5 cm in diameter and 5 cm in length using the experimental set-up
shown in Fig. 1. The average values of porosity and permeability of the
samples were 21% and 500 mD. Some samples were exposed to
different saturation periods (one week to one month) to analyze the
effect of aging on the diffusion process. Details of the experiments are
given in Table 2.
As the rst step, cores were prepared by cutting at the desired
length and diameter. Attention was paid to ensure that the rock
properties were consistent. This was achieved by choosing the
samples from the same block and orientation. Rock samples were
used for only one experiment to avoid any wettability change due to
Table 1
Fluid pairs used in the 2-D visualization experiments.
Pentane Kerosene
Density (g/cc) 0.63 0.79
Viscosity (cp) 0.38 2.9
33
(b)
Computer
Camera
Model
MicroPump
Light source
the core cleaning process. Counter-current interaction was obtained
by coating all sides of the sample except the bottom with epoxy
(Fig. 1-b).
Kerosene and mineral oil were chosen as the oil types and n-heptane
was used as the solvent phase in core experiments. The properties of
the uids are given in Table 3.
Prepared cores were saturated with kerosene or mineral oil in the
vacuum chamber for 48 h and pore volumes were determined from
the weight difference. Miscible interaction prevents visually identi-
fying the recovered oil. Therefore, the experiments were performed
using accurate scales (Fig. 1-a). The weight difference was translated
into recovered oil using a simple material balance equation. Interpola-
tion techniques were used for smoothing the errors. The n-heptane level
was kept constant in the tubes by continuous feeding using a micro-
pump (Fig. 2).
For some of the cores and 2-D visual models, different aging times
were applied for the mineral oil experiments. In earlier works
(Hatiboglu and Babadagli, 2007; 2008a), the same process for the
same oil altered the wettability to some extent as proven by changing
spontaneous water imbibition rates. In the present work, there is no
aqueous phase in the system (as initial water or water from a pre-
ush) and the process is a diffusive mass transfer of fully miscible
uids. Hence, what is tested is only the aging period of the sample
(rather than wettability) and its effect on the miscible interaction.
The recovery curves from the core experiments along with the
equivalent 2-D sand pack visual results are given in Figs. 511. Note
that the experiments conducted in this study were at zero initial
water saturation which is not representative of reservoir conditions.
3. Observations, results and analysis
Visualization experiments were coupled with core experiments to
explain the dynamics of the matrix fracture interaction. Displacement
patterns and the progress of the front obtained from the visualization
experiments, as well as the oil recovery curves of the core experiments
were the main concerns in this qualitative analysis.
Two different glass-bead models were constructed. The rst was a
three-side-sealed model to obtain fully counter-current ow and the
Mineral oil
second was a two-side-sealed model that provided a co-current ow.
0.83 Experiments were performed on vertically situated samples to
36.32
account for the gravity effect, as well as in a horizontal conguration.
34 C.U. Hatiboglu, T. Babadagli / Journal of Petroleum Science and Engineering 74 (2010) 3140

Table 2
Experiment identication according to core shape and rock type.

Cores 2-D sand packs

Shape Cylindrical Shape Square

Length (cm) 5 Dimensions 5 5 0.03 cm
Diameter (cm) 5
Vertical experiments (Counter-current) Fig. 5 (Mineral oil) Vertical experiments (Counter-current) Fig. 5 (Mineral oil)
Reference (unaged) V1
Exp. 14 (1-week aged) Fig. 6 (Mineral oil)
Exp. 19 (1 month aged) V1a
Fig. 7 (Mineral Oil) Fig. 7 (Mineral oil)
Mineral oil V2
Kerosene
Vertical experiments(Co-current) Fig. 7 (Mineral oil) Vertical experiments (Co-current) Fig. 8 (Mineral oil)
Mineral oil V3
Kerosene Fig. 9 (Mineral oil)
V4
Horizontal experiments (Counter-current) Fig. 11 (Mineral oil) Horizontal experiments (Counter-current) Fig. 11 (Mineral oil)
Mineral oil H1
Fig. 12 (Mineral oil)
H2
Horizontal experiments with lter paper (All sides open) Fig. 3 (Mineral oil)
Horizontal experiments with lter paper (Counter-current) Fig. 4 (Mineral oil)
Horizontal experiments (Co-current) Fig. 13 (Mineral oil)
H3
Fig. 14 (Mineral oil)
H4
Inclined experiments (Counter-current) Fig. 15 (Mineral oil)
I1
Fig. 16 (Mineral oil)
I2

The effect of the oil viscosity and density on the process was also
considered using two different types of oil.
3.1. Vertical experiments: counter-current interaction
Two different oil types, kerosene and mineral oil, were compared
in Figs. 57 for counter-current experiments in a vertical direction.
The difference in aging was also considered in Figs. 5 and 6.
Compared to the mineral oil (Fig. 5-c), the kerosene experiment
was much faster and generated slightly thinner ngers (Fig. 7-c). The
front reached the top boundary much earlier in the kerosene. Then,
the process was controlled predominantly by gravity due to the
density difference between the original oil (higher density) and the
mixture (solvent and the original oil) which has lower density. This
was reected on the recovery curves (the triangles in Fig. 7-a) as a
bump (see the change in the slope of the recovery curve at 0.4 OOIP
original oil in place recovery). Because of this, oil production was
initially faster for the kerosene.
It was observed that the pressure distribution created by boundary
conditions inside the porous medium model (inner pressure) and
gravity played a signicant role on the displacement front. This was
also observed in our computational studies (Hatiboglu and Babadagli,
2008b) where the process studied experimentally in the present
paper was stochastically modeled and pressure distributions inside
the models created by the boundary conditions were illustrated. It is
notoriously hard to construct a at and homogeneous 2-D glass-bead
pack. We followed the same procedure in the model preparation and
assumed that the beads were packed with similar efciency. Vertically
positioned models showed a convective displacement mechanism
regardless of the oil type. The uid fronts tend to progress through the
sides of the model where less resistance exists compared to the center
due to an existing inner pressure distribution. Once the gravity driven

Fig. 3. Mineral oilpentane diffusion on a lter paper (all sides open, horizontal).

Fig. 4. Mineral oilpentane diffusion on a lter paper (horizontal, counter-current only bottom part is open to ow and process progressing upwards).
 C.U. Hatiboglu, T. Babadagli / Journal of Petroleum Science and Engineering 74 (2010) 3140 35

Table 3 tion/waste disposal in which the matrix portion is desired to be the

Properties of the uids used in the core experiments.
Properties Mineral oil
Density (g/cc) 0.83
Viscosity (cp) 36.32
front reaches the top of the model, lighter components start to
accumulate over the heavier component, pushing the heavier oil
phase down. This can be called buoyant convection where
displacement develops through the sides of the sample and goes
downward from the inner part.
For the less viscous kerosene, this effect was more signicant. The
kerosene saturated sample had an advantage in terms of the oil
recovery rate even though the gravitational (buoyancy) force is
expected to be much lower (because of the mineral oil and kerosene
density difference); a low viscous nature of the oleic phase makes it
easier for the solvent to disperse (Fig. 7-a).
Kerosene, lighter in terms of density and with a lower viscosity,
showed more ngering but eventually a better sweep. The integrity
within the ngers was preserved. Lower viscosity translates as better
dispersion of the solvent through higher ow speed due to gravity.
Note that the convective transport rising from the edges (due to
gravity) of the model and descending from the middle portion caused
re-production of the solvent. This could be a critical issue in processes
like CO2 sequestration in oil reservoirs and contaminant transporta-
storage medium holding the solvent (or injected) phase.
n-Heptane An aged sample (Fig. 6) showed a similar behavior compared to
the non-aged one (Fig. 5-c). The process time and dynamics were
0.67
0.42 quite similar except that the unswept zones were slightly larger for a
given time in the case of the aged sample as also reected by
lower recovery at any time on the recovery curves (Exps. 14 and 19 in
Fig. 5-a) compared to the unaged case (indicated as Reference in
Fig. 5-a). Note that the convective process was also observed and
eventually the whole sample was swept in a longer time compared to
the non-aged sample. The convective transport due to gravity was
observed to be more prominent in the aged samples. The aged case
(Fig. 6) presented smoother displacement fronts with less nger
compared to the non-aged case (Fig. 5).
3.2. Vertical experiments: co-current interaction
When the co-current models of vertical orientation were used, two
distinctive patterns were obtained for the mineral oil and kerosene
cases (Fig. 8 and 9). Pressure distribution altered with the top edge
open to the atmosphere and this caused different displacement fronts
compared to the counter-current interaction. The kerosene case
showed convection type displacement similar to the counter-current
cases given above with a more distinctive ngered pattern which
translates into signicant bumps on the recovery curve (triangles in

(a) (b)
100%
Reference
9 Repeatibility 80%
14-(1Week Aged)
Recovery (OOIP)

19-(1Month Aged)
60% Samples
saturated
with Mineral
40%
Oil

20%
interaction
0% from bottom
1 10 100 1000 10000 100000 of the
Time (min) sample

(c)

Fig. 5. Experiment V1 (counter-current, mineral oil) (a) recovery curve for core experiment, (b) schematic representation of core and 2-D model, (c) 2-D visualization experiment (darker
color corresponds to solvent, lighter one is oil). OOIP: Original Oil in Place, reference: original (unaged sample), repeatability: repetition of the reference case on a different core sample.

Fig. 6. Visualization experiment for the aged sample, V1a: Counter-current, mineral oil. Darker color corresponds to solvent, lighter one is oil.
36 C.U. Hatiboglu, T. Babadagli / Journal of Petroleum Science and Engineering 74 (2010) 3140

(a) (b)
Counter-Current, Vertical
100%
Kerosene
80%
Recovery (OOIP)

Mineral Oil
Sample
60% saturated
with
40%
Kerosene

20%
interaction
from bottom
0% of the
1 10 100 1000 10000 100000
sample
Time (min)

(c)

Fig. 7. Experiment V2 (counter-current, kerosene) (a) recovery curve for core experiment, (b) schematic representation of core and 2-D model, (c) 2-D visualization experiment
(darker color corresponds to solvent, lighter one is oil). OOIP: Original Oil in Place.

Fig. 9-a, rst bump at 0.45 OOIP and the second at 0.8 OOIP recovery).
The uid front progressed faster near the two edges and accumulation
at the top boundary started after 32 min for the kerosene (Fig. 9). In
the core experiments, the effect of buoyant convection (accumula-
tion) starts to appear around 25 min (that is the point where the curve
shows a bump and inclination starts). The light color in the center of
the model indicates some residual oil saturation in the middle portion.
The experiments done with the mineral oil showed a totally
opposite behavior, where the bullet shaped displacement front is
centered along the model without any signicant ngering (Fig. 8-c).
This indicates that viscosity dominates over the gravity effect. The
front was much more stable than that of kerosene in the same model
conguration. The inner pressure distribution (higher resistance to
ow near the sides and less resistance in the middle portion of the

(a) (b)
Co-Current , Vertical
100%
Open to atmosphere
Kerosene
80%
Samples
Recovery (OOIP)

Mineral Oil
saturated
60%
with
Kerosene
40% or Mineral
Oil
20%

0% interaction
1 10 100 1000 10000 100000 from bottom
Time (min) of the
sample
(c)

Fig. 8. Experiment V3 (co-current, mineral oil) (a) recovery curve for core experiment, (b) schematic representation of core and 2-D model, (c) 2-D visualization experiment (darker
color corresponds to solvent, lighter one is oil). OOIP: Original Oil in Place.
 C.U. Hatiboglu, T. Babadagli / Journal of Petroleum Science and Engineering 74 (2010) 3140
Fig. 9. Experiment V4 (co-current) 2-D visualization experiment with kerosene. Darker color corresponds to solvent, lighter one is oil.
model) and viscosity were the dominant factors controlling the
process. Once the front reached the top, the gravitational forces
started to become effective and the convective transport started. The
displacement efciency was much lower than that of the kerosene
yielding some unswept zones as can be seen through the comparison
of Figs. 8 and 9.
It was very obvious that the dispersion of the solvent phase (due to
gravity) was more prominent in the case of kerosene. This apparently
caused more efcient displacement of oil compared to the mineral oil.
In other words, the dispersive ow is more pronounced in the case of
kerosene due to low viscosity and less resistance to ow, causing a
more effective convective transport. This can be attributed to the
lower viscosity of kerosene compared to mineral oil.
Four experiments comparing two different uids and two different
orientations are plotted in Fig. 10. The shapes of the curves conrm
that ngering is an indication of faster recovery. In fact, kerosene
exhibited more ngering for all cases compared to mineral oil. This
was more obvious for the co-current interaction (compare Figs. 7
and 9). This is reected as faster recovery on the recovery curve. With
the mineral oil, changing the boundary conditions from counter-
current to co-current caused the ngers to disappear and the process
continued as bulk diffusion for long time, then converted to
convective ow. This behavior is also traceable from the recovery
curves where the rate of oil for mineral oil is lower. The bumps on the
kerosene recovery curves are obvious and this is attributed to quicker
arrival of the front at the top of the model due to severe ngering.
3.3. Horizontal experiments: counter-current interaction
Horizontal orientation showed a steady and frontal displacement
for all cases (Figs. 11 and 12). Counter-current experiments yielded a
bullet shaped front prole as the gravity was not in effect. At early
stages, a random process was observed in the shape of ngers,
Vertical
Recovery (OOIP)
1 10 100 1000 10000
Time (min)
Kerosene - Co-current Mineral Oil - Co-current
Kerosene - Counter-current Mineral Oil - Counter-current
Fig. 10. Comparison of the four experiments given in Figs. 59. (OOIP: Original Oil in
Place).
37
conrming that the process is diffusion dominated for a short period
of time. The nger development was similar to the lter paper
experiments (Figs. 3 and 4). This indicates that the horizontal process
is more of a stochastic process but the pattern would be highly
dependent on pore structure and homogeneity rather than matrix
boundary conditions and uid type in the later stage. The develop-
ment and progress of the front for the mineral oil and kerosene cases
were quite similar. Obviously, the process of time for the mineral oil
was much longer as indicated in Figs. 11 and 12. This can be explained
by a slightly lower diffusion coefcient and higher viscosity of the
mineral oil.
The comparison of the recovery curves for horizontal and vertical
positioning indicated that the gravity driven vertical process is much
faster (Fig. 11-a). Buoyancy caused by the density difference and
gravity helps the solvent phase disperse into the heavier oil phase,
increasing the recovery rate. This is especially signicant for the low
viscosity kerosene. It is interesting to note that the bumps on the
curves were not observed in either case unlike the recovery curves for
kerosene.
3.4. Horizontal experiments: co-current interaction
Difculties inherited due to the 3-D nature of the cores made it
highly difcult to conduct accurate and identical core experiments to
the 2-D visualization models. Therefore, it was only possible to provide
visualization experiments for horizontal co-current models. Co-current
experiments with one end open to the atmosphere had different
pressure distributions within the model (Figs. 13 and 14) compared to
the counter-current case. The displacement front preferentially pro-
gressed near the sides of the model, but no convective behavior was
observed due to a lack of gravity and buoyancy effects for both cases.
Mineral oil (Fig. 13) displayed a more stable front compared to the
kerosene due to its higher viscosity (Fig. 14).
3.5. Inclined experiments: clarication on the effect of gravity
Visualization experiments slightly tilted (10) from the horizontal
100%
orientation were performed to observe the effect of gravity (Figs. 15
and 16). Although the angle of orientation was only 10, it was
80% sufcient to observe the dominancy of the gravity effect and the
transformation of the process to convection. The difference between
60% the mineral oil and kerosene cases for the vertical and inclined
experiments is signicant in both process time and ngering behavior.
40% Shorter and thicker ngers are visible in both cases for the mineral oil
(Fig. 15) due to higher viscosity. Similar to previous cases, kerosene
20% yielded thinner and longer ngers and a much faster process.
Convective ow was observed to be more signicant in the case of
kerosene as similar to the vertical experiments.
0%
100000
4. Quantitative analysis
The process in the experiments is governed by diffusion mim-
icking the matrixfracture interaction under static conditions.
Therefore, the recovery curves given in the paper are controlled by
the parameter called effective diffusion coefcient (De). A logarithmic
relationship between time and effective diffusion coefcient was
38 C.U. Hatiboglu, T. Babadagli / Journal of Petroleum Science and Engineering 74 (2010) 3140

(a) (b)
Mineral Oil, Counter-Current
100%

Horizontal
80%
Recovery (OOIP)

Vertical
interaction
60% Sample from side of
saturated the sample
40% with Mineral
Oil
20%

0%
1 10 100 1000 10000 100000 1000000
Time (min)

(c)

Fig. 11. Experiment H1 (mineral oil) (a) recovery curve for core experiment, (b) schematic representation of core and 2-D model, (c) 2-D visualization experiment (darker color
corresponds to solvent, lighter one is oil). OOIP: Original Oil in Place.

Fig. 12. 2-D visualization experiment with kerosene, H2: Horizontal and counter-current case. Darker color corresponds to solvent, lighter one is oil.

observed (Wen et al., 2005). Using this approach, one expects that
the loglog plots of the recovery curves will yield a straight line and
the slope will give an effective diffusion coefcient for the particular
uid and rock properties.
The effective diffusion coefcient would depend on the solvent
viscosity ( s) and density (s), oil viscosity ( o), density difference
between oil and solvent (), solvent/oil diffusion coefcient (DF),
matrix porosity () and permeability (k), length (L) and diameter of
the core (d), which were the variables in our experiments. To obtain a
correlation between De and those variables, a multivariate regression
analysis was applied. In addition to the Berea sandstone core ex-
periments given in Table 1, a few limestone cases and one kerosene-
sandstone case reported previously by Hatiboglu and Babadagli (2008a)
were added. All the experiments considered in the development of

Fig. 13. 2-D visualization experiment with mineral oil, H3: Horizontal and co-current case. Darker color corresponds to solvent, lighter one is oil.

Fig. 14. 2-D visualization experiment with kerosene, H4: Horizontal and co-current case. Darker color corresponds to solvent, lighter one is oil.
 C.U. Hatiboglu, T. Babadagli / Journal of Petroleum Science and Engineering 74 (2010) 3140 39

Fig. 15. 2-D visualization experiment with mineral oil, I1: Inclined (10) and counter-current case. Darker color corresponds to solvent, lighter one is oil.

Fig. 16. 2-D visualization experiment with kerosene, I2: Inclined (10) and counter-current case. Darker color corresponds to solvent, lighter one is oil.

the correlation are given in Table 4. Note that all the experiments
represent a counter-current type interaction.
To correlate the effective diffusion coefcient obtained by measuring
the slope of the loglog recovery curves (second column of Table 4) to the
parameters given in the same table, we rst tested different dimension-
less groups listed by Trivedi and Babadagli (2008a). The following
equation was found to be the best correlation for counter-current
interaction after applying the multivariable regression analysis:
 b  c    e
o km L d
De = a
s tDF d/ S displacement in the vertical direction, especially for the co-current
where DF is the solvent (n-heptane) diffusion coefcient (6105 cm2/s),
and t is the time to reach the ultimate recovery obtained from the
recovery curves. That is the point at which the recovery curve reached
the plateau. Other parameters are dened in Table 4. Subscripts o and
s denote oil and solvent, respectively. The coefcients in Eq. 1 are
as follows: a=23.106, b=0.784, c=0.141, d=0.02, and e=0.714.
A comparison of the experimental and calculated (Eq. 1) values of
the effective diffusion coefcient is given in Fig. 17.
5. Conclusions and remarks
Miscible interaction between oil saturated rock and solvent
saturated fractures driven by diffusion and natural convection (or
buoyancy) for different uids, boundary conditions, orientations, and
sample aging times was studied for static conditions experimentally.
Two different methodologies were applied to study the mechanism,
visual 2-D models and real rock 3-D experiments. Then, the mechanics
of displacement by solvent diffusion and oil recovery through this
process were analyzed.
Vertically positioned models showed buoyant convective
type displacement caused by gravity and this accelerated the inter-
action process. Visual verications are supported with the recovery
curves obtained from corresponding core experiments. Depending on
the uid properties (characteristically viscosity), the displacement
process might diverge from convective to frontal displacement. The
mineral oilpentane diffusion case was the typical example for this
situation.
Viscosity and orientation were observed to be critical on ngering.
The most signicant ngering was obtained in the kerosene-pentane
1
models. For both the co- and counter-current cases, convective
displacement was observed. This was more severe for the co-current
interaction than for the kerosene case.
Horizontal experiments were diffusion dominated, dependent on
the boundary conditions of the model. The fronts proceeded randomly
through the easy ow zones (edges of the model) for co-current
interaction. In the case of counter-current interaction, bulk diffusion
type displacement yielding a frontal progress was obtained. Oil
recovery was slower compared to the vertical orientation and no
ngers were observed especially in the later stages of the process.
Apart from the visual experiments, different matrix dimensions
(shape factors) and aging times were tested through core experi-
ments. It was observed that for each type of rock, uncoated samples
gave the fastest recovery. Introducing boundaries changed the
interaction dynamics. To clarify the effect of aging on the process, a
few samples were exposed to different aging times. The aged Berea
samples showed similar trends and ultimate recoveries to the unaged
cases regardless of the core dimensions.
Finally, the effective diffusion coefcients for each case were
obtained through the slope of a loglog relationship between time

Table 4
Experimental data from the core experiments used in the development of effective diffusion coefcient correlation.

Experiment De L d M o S O S t-recovery kM
(in) (in) (cp) (cp) (g/cc) (g/cc) (104 min) (mD)

MOSS 9.0877 2 1 0.21 36.32 0.42 0.83 0.67 7.67 500

MOSS 7.9122 6 1 0.21 36.32 0.42 0.83 0.67 8.24 500
MOSS 9.7236 2 2 0.21 36.32 0.42 0.83 0.67 8.35 500
MOSS 8.6545 6 2 0.21 36.32 0.42 0.83 0.67 8.21 500
MOLS 4.4461 2 1 0.17 36.32 0.42 0.83 0.67 9.18 12
MOLS 6.5534 6 1 0.17 36.32 0.42 0.83 0.67 9.27 12
MOLS 4.9922 2 2 0.17 36.32 0.42 0.83 0.67 9.15 12
MOLS 4.8469 6 2 0.17 36.32 0.42 0.83 0.67 9.09 12
KSS 0.9686 2 2 0.21 2.9 0.42 0.79 0.67 8.34 500

MO: mineral oil, SS: sandstone, LS: limestone, K: kerosene, t-recovery: time to reach the ultimate oil recovery, kM: matrix permeability, o: oil viscosity, o: oil density, s: solvent
viscosity, s: solvent density, and : porosity of matrix.
40 C.U. Hatiboglu, T. Babadagli / Journal of Petroleum Science and Engineering 74 (2010) 3140

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