A magnetic resonance study of pore lling processes during spontaneous

imbibition in Berea sandstone

Quan Chen
MRI Centre, Department of Physics, P.O. Box 4400, University of New Brunswick, Fredericton,
New Brunswick E3B 5A3, Canada
Murray K. Gingras
Department of Earth and Atmospheric Sciences, University of Alberta, Edmonton, Alberta T6G 2E3, Canada
Bruce J. Balcom
a)
MRI Centre, Department of Physics, P.O. Box 4400, University of New Brunswick, Fredericton,
New Brunswick E3B 5A3, Canada
Received 16 May 2003; accepted 13 August 2003
A new magnetic resonance technique, DDIF the decay of magnetization due to diffusion in the
internal eld, was combined with mercury porosimetry to investigate pore geometry, including
pore- and throat-size distribution, and pore connectivity for porous media. A comparison of DDIF
spectra for a fully water saturated Berea sandstone, with the partially saturated sample by
centrifugation in air, indicated that DDIF can be used for the measurement of water lled pore size
distribution in partially saturated porous media. Dynamic water imbibition into air-lled Berea
sandstone was studied using the DDIF technique. Simultaneously, in situ three-dimensional
saturation and capillary driven water penetration were monitored using Conical-SPRITE, which is
a rapid, centric scanning, spin-density weighted single point three-dimensional magnetic resonance
imaging technique. These measurements provide direct evidence for differences in the pore lling
mechanisms for co-current imbibition and counter-current imbibition in Berea sandstone. During
co-current imbibition, water ows through the pores and connected throats with a piston-type
mechanism. Air is displaced from the sample by the leading edge of the waterfront, resulting in a
macroscopic piston-like ow through the entire sample. During counter-current imbibition, water
ows through the pores and connected throats with a lm-like structure along the corners and
surfaces of the pore space. Air escapes from the sample by owing through the center of the pores
and pore throats, in the opposite direction. Once the penetrating waterfronts meet, at the sample
center, there is a global, uniform increase in water content. 2003 American Institute of Physics.
DOI: 10.1063/1.1615757
INTRODUCTION
Spontaneous imbibition is the process by which a wet-
ting uid is drawn into a porous medium by capillary action.
Co-current and counter-current imbibition are dened as
wetting and nonwetting uid ow in identical, and opposite
directions, respectively. The imbibition effect is critical to oil
recovery from sedimentary reservoirs, especially those reser-
voirs which are fractured.
1
Ground-water ow in porous me-
dia in unsaturated layers is also related to the imbibition
effect.
2
Thus, studies of imbibition have received consider-
able attention in the literature. Morrow has thoroughly dis-
cussed the inuence and importance of imbibition for oil
recovery.
3
Imbibition mechanisms have been studied using model
capillary tube networks. Fluid imbibition into capillary tubes,
with triangular
4
and square
5
cross sections, provide a varia-
tion on the basic case of the cylinder. Lenormand et al.
6
has
undertaken fundamental work on the mechanisms of immis-
cible displacement in capillary micromodel networks with
rectangular ducts.
A piston-like displacement for co-current imbibition
7
and more diffuse imbibition fronts for counter-current
imbibition
8
have been observed by x-ray CT in porous me-
dia. However, in the absence of direct measurements of pore-
and throat-lling processes during imbibition in porous me-
dia, it has not been possible to verify the suggested co-
current imbibition mechanism at the pore level. Furthermore,
the pore-level mechanism of counter-current imbibition in
porous media is still not clear.
The internal space of porous media is usually described
as a series of cavities pores connected by smaller channels
pore throats or throats.
1
In this paper we combine DDIF
the decay of magnetization due to diffusion in the internal
eld
9
with mercury porosimetry to obtain detailed and quan-
titative pore geometry information for the Berea sandstone.
The processes of spontaneous co-current and counter-current
imbibition, as well as water displacement by air using cen-
trifugation, were monitored by DDIF and three-dimensional
3D Conical-SPRITE magnetic resonance imaging MRI.
10
Dynamic ow processes were monitored by DDIF water-
a
Author to whom correspondence should be addressed. Electronic mail:
bjb@unb.ca
JOURNAL OF CHEMICAL PHYSICS VOLUME 119, NUMBER 18 8 NOVEMBER 2003
9609 0021-9606/2003/119(18)/9609/8/$20.00 2003 American Institute of Physics
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lled pore-size distribution measurements, while the in situ
3D water content was detected by 3D Conical-SPRITE MRI
during spontaneous imbibition. Different pore- and throat-
lling mechanisms were revealed for co-current imbibition
and counter-current imbibition in natural porous media.
THEORY
A recently developed NMR method based on the decay
of magnetization due to diffusion in the internal eld
DDIF
9
was used to determine the pore size
11
and pore
geometry
12
in Berea sandstone.
Since the DDIF method is relatively new, we will outline
the basic theory of the method. When a uid-lled porous
medium is subjected to a uniform magnetic eld, a spatially
varying eld, and its gradients, appear inside the pore space
due to susceptibility differences between the solid and
the pore-lling uid.
1315
This susceptibility-induced gradi-
ent is called the internal gradient, and it may be very strong,
especially in sedimentary rocks.
16
The internal gradient de-
pends on the geometry of the pore space. Variations of the
internal gradient in the pore space are a reection of the pore
size change in porous media.
The diffusion of longitudinal nuclear spin magnetization
is governed by the TorreyBloch equation
17

t
m r, t D
2
m r, t m r, t . 1
Here, D is the bulk diffusion coefcient, is the bulk
spin relaxation rate, and m is the deviation of the magnetiza-
tion from its equilibrium value.
A solution of the equation can be expressed in the gen-
eral form
m r, t e
t

n0
n
a
n

n
re
t/
n
, 2
where
n
and
n
are eigenfunctions and eigenvalues, the
index n refers to the mode number, a
n
is intensity of each
mode. The eigenvalues are determined by the boundary con-
dition: Dn

n
, where n

is the unit vector normal to

the surface and the surface relaxivity. The decay rate of the
lowest mode is associated with the surface-to-volume ratio
S/V and is approximately S/V. The higher modes are
less sensitive to surface relaxivity
18
and diffusive coupling
effects between interconnected pores
19
and depend primarily
on pore geometry.
The pulse sequence used for DDIF is the stimulated
echo
21
/2t
e
/2t
d
/2t
e
echo. 3
The symbol /2 represents a radio-frequency RF pulse
that rotates the spin vector by 90 degrees, t
e
is the encoding
time while t
d
is the diffusion time. After the rst t
e
, a
position-dependent phase difference between spins is created
due to the inhomogeneity of B
i
(r), the local magnetic eld.
The phase differences of spin magnetization encoded by
the internal eld B
i
(r) are: B
i
(r)t
e
, where is the
gyromagnetic ratio. A four-step phase cycling for the DDIF
sequence is employed as in Ref. 20. A 90 degrees phase
difference between the rst two pulses was chosen, in order
to select the sine part of the phase modulation due to the
internal eld during the rst t
e
. Thus, the magnetization m
after the second pulse is given by
mm
0
sin , 4
where m
0
is the initial magnetization before the rst pulse.
After the second /2 pulse, the spatially dependent
phase differences are encoded as a spatial pattern of ampli-
tudes of spin magnetization. During t
d
, spins undergo mo-
lecular self-diffusion and spin-lattice relaxation. After a sec-
ond t
e
, the spin position is decoded with the identical
internal eld B
i
(r). An echo signal is acquired at time t
e
after the third pulse. The experiment is performed for a series
of t
d
times. We use a regime of weak phase encoding where
the rst eigenmode (n1) is predominantly excited, so the
signal of the rst mode is linearly proportional to the encod-
ing phase, and the pore size distribution is determined by the
DDIF spectrum.
20
A reference pulse sequence is used to calibrate the
effect of spin-lattice relaxation during t
d
: /2t
e

t
e
/2t
d
/2FID. Here the symbol denotes an RF
pulse that rotates the spin vector by 180 degrees. The pulse
is used to cancel the phase accumulation due to internal gra-
dients, so the free induction decay FID signal measures
only the effect of spin-lattice relaxation. An eight-step phase
cycling was used for the reference sequence.
20
The DDIF and reference decay curves are shown in Fig.
1. Compared to the reference signal, the fast decay rate for
the DDIF data at short t
d
is due to molecular diffusion
through B
i
which varies over the pore length scale. At long
t
d
, when the diffusing molecules have traversed all of the B
i
space in the pore, the decay due to diffusion ceases, and E
and R decay at a similar rate. Therefore, the DDIF is a direct
reection of pore geometry.
In the fast diffusion limit, the measured DDIF echo E
and Reference FID R signal can be expressed as
9
R t
d
e
t
d
/
0
, 5
E t
d
a
0
e
t
d
/
0

n1

a
n
e
t
d
/
n
. 6
FIG. 1. DDIF E and reference R signals as a function of t
d
for the Berea
sandstone. A more rapid decay of the DDIF signal is observed at short t
d
,
due to the effects of diffusion through internal gradients. The decay curves
of DDIF and reference signals are parallel at long t
d
.
9610 J. Chem. Phys., Vol. 119, No. 18, 8 November 2003 Chen, Gingras, and Balcom
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The intensity of the lowest mode (a
0
) is determined by
the ratio of E(t
d
) and R(t
d
) at a long t
d
, and its contribution
to E(t
d
) can be subtracted. An inverse Laplace transform
was carried out with the data of E(t
d
)a
0
R(t
d
) to yield the
DDIF spectrum.
Under fast diffusion conditions, the pore size distribution
can be obtained using the following equation:
22

n
4r
2
/Dn
2

2
, n1,2,3. 7
Here
n
are eigenvalues, r is pore radius, D the bulk diffu-
sion constant, the index n refers to the mode number.
When the porous media is only partially saturated, the
air may occupy the pores fully or partially. In the partially
saturated pores, they are always more waterwet than air
wet. The water spreads on the surface of the pore space,
while the air occupies the pore center. The susceptibility SI
unit values of our samples are:
16
Berea89.8510
6
,
water9.0510
6
, air0.3610
6
. As the sus-
ceptibility difference between Berea sandstone and air is
similar to the difference between Berea sandstone and water,
we assume that the internal eld distributions in the water
phase in partially saturated porous media resemble these of a
fully saturated sample.
Three dimensional water content images employed
Conical-SPRITE,
10
which is a rapid, 3D, centric k-space
sampling,
23
spin-density weighted single point imaging tech-
nique. Like other single point imaging
24
techniques, Conical-
SPRITE is free from the distortions due to chemical shift,
susceptibility variations, and B
0
-inhomogeneity. Compared
with the standard SPRITE single-point ramped imaging
with T
1
enhancement
25
method, Conical-SPRITE has many
advantages, such as fast acquisition speed, low duty cycle
and reduced sensitivity to T
1
.
The Conical-SPRITE technique uses a conical k-space
scanning trajectory starting from the center of k-space with
three ramped phase-encoding gradients. The pulse sequence
is illustrated in Fig. 2. The actual sampling of k-space is
discrete, with gradient amplitudes calculated to ensure the
sampled points fall on a Cartesian grid. A conventional FFT
may be applied for image reconstruction.
In the Conical-SPRITE method, the observable local
sample magnetization M is given by
MM
o
e
t
p
/T
2
*
sin , 8
where M
o
is the equilibrium magnetization, t
p
is the phase
encoding time, T
2
* is the effective spinspin relaxation time,
and is the ip angle. Conical-SPRITE is naturally spin-
density weighted. From this signal equation, as long as t
p
T
2
* , or if T
2
* is a constant in the sample, the only factors
impacting the intensity of signal observed are the local equi-
librium magnetization, M
o
, which is proportional to local
water content, and the ip angle, .
For a Conical-SPRITE image with matrix size N
3
, a
eld of view FOV, maximum phase encoding gradient value
of G
zMax
, the nominal pixel resolution (z) will be
z
FOV
N

G
zMax
t
p
. 9
The low duty cycle advantage of the Conical-SPRITE
technique may allow the use of a stronger gradient to in-
crease resolution, or the use of a shorter t
p
for increased
spin-density weighting, and decreased T
2
* weighting. The
minimum t
p
is limited by the maximum gradient strength
and the instrument deadtime; t
p
is typically tens of microsec-
onds.
EXPERIMENT
Berea sandstone samples were used for the experiments.
Its porosity the ratio of pore volume to bulk volume of rock
was 18.6%, and permeability 0.18 m
2
. The sample for im-
bibition and centrifugation, as well as NMR experiments,
was 25 mm in diameter and 52 mm in length. The sample for
mercury intrusion was 25 mm in diameter and 25 mm in
length. All experimental samples were extracted from the
host rock in close proximity to one another. They have a
similar pore structure due to the homogeneity of the Berea
sandstone formation. All samples were dried at 80 C until
constant mass was achieved.
The sample was fully saturated under vacuum conditions
for DDIF and 3D Conical-SPRITE imaging to determine
baseline information on the pore geometry and porosity dis-
tribution. Then, the process of desaturation was performed
with a Model J2-21 centrifuge with JA-14 rotor Beckman
Instruments, Inc. at a constant temperature 4 C to avoid
evaporation during centrifugation. The sample was centri-
fuged at a constant rotational speed of 2500 RPM this cor-
responds to a centrifugal force of 0.16 MPa at the center of
the core for one hour and then 7000 RPM this corresponds
to a centrifugal force of 1.27 MPa at the center of the core
for an additional hour. DDIF experiments were carried out
after each centrifugation.
Following centrifugation, the sample was dried once
more. Spontaneous imbibition experiments were performed
with distilled water. In the case of co-current imbibition, the
bottom of the rock sample was kept in contact with a bulk
water reservoir. For counter-current imbibition, the whole
sample was immersed in distilled water. The water was
drawn into the center of the core from the surface by capil-
FIG. 2. Conical-SPRITE MRI pulse sequence. Three phase-encoding gradi-
ents (G
x
, G
y
, and G
z
) are employed. Oscillating X and Y gradients, as well
as a ramped Z gradient dene a conical trajectory in k-space. An RF pulse is
applied at each gradient level. The repetition time TR is the time between
successive RF pulses, a single FID point is sampled at a time t
p
after each
RF pulse.
9611 J. Chem. Phys., Vol. 119, No. 18, 8 November 2003 Pore lling processes
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lary forces. Water saturation change versus time was mea-
sured gravimetrically. At different saturation states, DDIF
and 3D Conical-SPRITE MRI were carried out with the
sample sealed by Teon tape to avoid evaporation. The
sample was repetitively dried, and the procedure repeated
several times at different saturation states.
All NMR experiments were performed in a 2.4T hori-
zontal bore superconducting magnet Nalorac Cryogenics
Inc., Martinez, CA with an Apollo console Tecmag Inc.,
Houston, TX. The co-current imbibition dynamic process
was monitored by 3D Conical-SPRITE MRI with the rock
sample and water reservoir in the magnet, employing a
homemade single turn solenoid coil with a vertical orienta-
tion and 38 mm id. For all other NMR experiments, a proton-
free 47 mm inner diameter eight-rung quadrature birdcage
probe Morris Instruments, Ottawa, ON was employed.
For the DDIF experiments, the t
e
was 50 s, with a
series of 35 t
d
values chosen to span 10 s to 3 s logarith-
mically.
For Conical-SPRITE imaging, the imaging matrix was
646464, eld of view FOV was 7 cm7 cm7 cm,
ip angle of 13, phase encoding time (t
p
) of 40 s, and
repetition time TR of 2 ms, with 39 discrete cones sampled
for a single scan imaging time of only 2.5 minutes.
RESULTS AND DISCUSSION
Baseline information on the pore geometry and a 3D
porosity distribution were obtained with DDIF and mercury
porosimetry, as well as Conical-SPRITE MRI to determine
the samples heterogeneity at the pore level m and at the
voxel level mm, respectively.
Pore- and throat-size distribution and pore
connectivity
An overlay of the DDIF spectrum, for fully water satu-
rated sample, and mercury porosimetry results is shown in
Fig. 3. The amplitudes of the two distributions are calibrated
to saturation of the Hg and water separately. The DDIF spec-
trum shows a predominant peak at around 70 m, which is
consistent with the large number of pores with similar diam-
eter observed from the thin-section image, Fig. 4. A shoulder
in the distribution extends to a few m with a reduced am-
plitude.
It is well known that mercury intrusion porosimetry
yields throat-size distributions. The throat-size distribution
was obtained by measurement of the mercury intrusion cap-
illary pressure curve.
26
The result shows a single peak at
about 15 m with a very small shoulder down to a few m.
The mercury derived size distribution shows a peak at a size
much smaller than the dominant DDIF peak. This indicates
that the pore sizes represented by the dominant DDIF peak
are interconnected with throat sizes represented by the single
peak for the mercury experiment. The left shoulder of the
DDIF spectrum with a size range less than space 10 m, is
due to the rough surfaces and lining materials which are
shown in Figs. 4 and 5.
3D images of fully saturated sample
The free induction decay FID is frequently observed to
be single exponential in porous media, with the spinspin
relaxation time (T
2
) decay usually multiexponential. Proton-
density imaging is thereby readily obtained for the FID based
Conical-SPRITE imaging technique from Eq. 8 by single
exponential tting the FID data from a series of Conical-
SPRITE images with variable encoding times.
The semilogarithmical decay curve of Fig. 6 is observed
after a 90 degrees RF pluse. The data was t to the equation
SS
0
exp t/T
2
*. 10
Where S is the NMR signal intensity, S
0
is NMR signal
intensity at t0, t is the acquisition time, and T
2
* is the
effective spinspin relaxation time. The t T
2
* was 127 s.
The FID has a single exponential decay over 2 orders of
signal intensity. Similar results were obtained for all Berea
sandstone samples.
Experiment shows the T
2
* of the Berea sandstone
samples varied from 114 to 127 s in different imbibition
states with water saturation varying from 9.1% to 100%. For
FIG. 3. A comparison of the mercury porosimetry and DDIF spectrum for a
fully water saturated Berea sandstone. The amplitudes of the distributions
are scaled to the mercury Hg and water saturation Sw, respectively. The
peaks in the mercury porosimetry and DDIF spectrum indicate a throat size
of 15 m and pore size of 70 m.
FIG. 4. An optical micrograph of a thin-section of the Berea sandstone
sample. The white regions are pore space identied by the color of an
impregnated epoxy. The gray regions are large quartz crystals, and the dark
regions are small crystals and clay. The black scale bar is 70 m. Many
pores on the order of 70 m are apparent.
9612 J. Chem. Phys., Vol. 119, No. 18, 8 November 2003 Chen, Gingras, and Balcom
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3D Conical-SPRITE images with t
p
of 40 s, assuming the
term exp(t/T
2
*) is constant in Eq. 10, causes a relative
error of less than 3.5%. Under these experimental conditions,
3D Conical-SPRITE images are essentially proton-density
images.
2D longitudinal slice a and transverse slice b images
from 3D Conical-SPRITE images for the Berea sandstone
with water saturation of 100% are shown in Fig. 7. These
two slices are from the center of the core. They reveal a
homogenous porosity distribution of the sample.
Water displacement by centrifugation
As the mechanism of uid displacement in porous media
by centrifugation is well known, the comparison of DDIF
spectra between fully saturated Berea sandstone and the par-
tially saturated sample by centrifugation in air at different
angular velocities was undertaken as a control experiment. It
was intended to verify the validity of our previous assump-
tion that the internal eld distributions in the water phase in
a partially saturated sample resemble these of a fully water
saturated sample.
A comparison of the DDIF spectra between a fully water
saturated sample and desaturated sample by centrifugation is
shown in Fig. 8. In this gure, r is the radius of pores and
throats. The amplitudes of the DDIF spectra were scaled to
the water saturation Sw. After centrifugation for one hour,
2500 RPM, the average water saturation was 31.3%. Almost
all of the large pores (r30 m) have been emptied and are
not observed in the DDIF spectrum after centrifugation. This
indicates that these large pores must be interconnected with
the large throats whose capillary forces are less than the cen-
trifuge force.
After centrifugation for another hour, 7000 RPM, the
average water saturation decreased to 19.5%. The saturation
at a centrifugal force of 1.27 MPa should correspond to the
irreducible water saturation. A comparison of the two DDIF
spectra shows that water content in some relatively small
pores has changed. These pores must be connected by small
throats whose capillary forces are less than the centrifuge
force at 7000 RPM. The spectrum shows that the irreducible
water is distributed in very small pores which are connected
by even smaller throats.
After centrifugation, the left side of the DDIF spectra,
with length scale beyond the spectrum of full water satura-
tion, is likely due to residual water on the rough surfaces of
the pore space and in the pore lling materials, which ex-
FIG. 5. Environmental scanning electron microscopy ESEM measurement
for Berea sandstone. Rough particle surfaces and lling materials are appar-
ent. The black scale bar is 250 m in length.
FIG. 6. A semilogarithmical plot of the FID for the fully water saturated
Berea sandstone following a 90 degree RF pulse. The best t line is single
exponential with a decay time constant T
2
* of 127 s.
FIG. 7. A 2D longitudinal slice a, and transverse slice b, from a 3D
Conical-SPRITE MRI data set for the Berea sandstone with water saturation
of 100%. The images show a uniform porosity distribution of the Berea
sandstone sample. The FOV was 7 cm7 cm, and slice thickness was 1 mm.
FIG. 8. The DDIF spectra before and after centrifugation at rotation speeds
of 2500 RPM, and then 7000 RPM for one hour. The corresponding water
saturation Sw is 31.3% and 19.5%. The amplitude of each spectrum was
calibrated to the bulk water saturation.
9613 J. Chem. Phys., Vol. 119, No. 18, 8 November 2003 Pore lling processes
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changes rapidly with the water in the pores when the pores
are lled.
The comparison experiments of DDIF before and after
centrifugation indicates that DDIF can be used for the mea-
surement of water lled pore size distribution in partially
saturated porous media.
Co-current imbibition
To verify the piston-like displacement pattern proposed
in the literature, DDIF and Conical-SPRITE experiments
were combined to detect the pore lling processes and 3D
saturation evolution respectively during co-current imbibi-
tion.
A comparison of the DDIF spectra for full saturation,
and co-current imbibition for 30 minutes with water satura-
tion of 35.5%, as well as co-current imbibition for 13 hours
with water saturation of 57.9%, is shown in Fig. 9. The water
saturation did not increase with further imbibition once the
water saturation reached 57.9%.
The similar shape of the three DDIF spectra, at different
saturation states, indicates that during co-current imbibition,
water ows through the pores and connected throats with a
piston-like pattern.
The left side of the DDIF spectrum in Fig. 9, partially
saturated samples, reveals water occupancy in pore sizes
smaller than the corresponding fully saturated sample. This
is presumably due to water coating the pore lining materials,
or residing on the rough surfaces of the pore space.
The in situ saturation distribution during spontaneous
co-current imbibition is shown with the image series of Fig.
10. The broad base in the images is a water reservoir, the
weak signal observed at left in the images is background
signal from a plexiglass component in the RF probe. The
water signals in the Berea sandstone core show a rectangular
shape, and exhibit a piston-like water front movement. Be-
hind the advancing waterfront, no further increase of water
saturation was apparent. Water ow with this kind of piston-
like pattern on the macroscopic scale is due to water lling
the pores and connected throats uniformly, which was ob-
served by DDIF on the pore level.
Counter-current imbibition
As the dynamic process of counter-current imbibition is
more complex, and its microscopic mechanism is not clear,
we combined DDIF and 3D Conical-SPRITE experiments to
detect the imbibition processes in the Berea sandstone on a
pore-level and voxel-level, respectively.
An overlay of the DDIF spectra of full saturation and
spontaneous counter-current imbibition at different saturation
is shown in Fig. 11. The overall water saturation was 26.3%
after imbibition for 8 seconds. At the beginning of imbibi-
tion, the DDIF spectrum shows a very low saturation in
pores, and relatively higher water saturation in throats, due to
water ow through the pores and throats along the corners
and rough surface in the pore space with a lm-type struc-
ture. Air must ow along the center of the pores and throats
in the opposite direction due to the nature of water uptake in
the counter-current experiment. After counter-current imbibi-
tion for 84 minutes, the average water saturation was 56.0%.
The water saturation did not signicantly increase with fur-
ther imbibition, indicating that water saturation of 56.0% ap-
proximately corresponded to the nal imbibition equilibrium.
FIG. 9. The DDIF spectra during co-current imbibition at different water
saturation Sw levels. The amplitude of each spectrum was scaled to the
bulk water saturation. After co-current imbibition for 30 minutes, the overall
water saturation was 35.5%. After co-current imbibition for 13 hours, the
water saturation was 57.9%. The water saturation increased minimally with
further imbibition. The similar shape of DDIF spectra at different saturation
levels indicates that water ows through the pores and connected throats
with a piston-type mechanism.
FIG. 10. The dynamic process of co-current imbibition for the Berea sand-
stone observed by 3D Conical-SPRITE imaging. A series of images af
show 2D longitudinal slices from 3D Conical-SPRITE MRI data sets. The
time interval between the successive images was 10.5 minutes. The images
show a piston-like water penetration thereby implying a piston-like air dis-
placement from the open top of the sample. The at base in the images is a
water reservoir, the weak signal observed at left in the images is background
signal from a plexiglass component in the RF probe.
9614 J. Chem. Phys., Vol. 119, No. 18, 8 November 2003 Chen, Gingras, and Balcom
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The DDIF spectrum still shows a lower saturation in the
pores, compared with co-current imbibition, due to water
bubbles trapped in the center of pores. The left side of the
DDIF spectra, with length scale beyond the spectrum of the
full water saturation, is due to water lling the pore lining
materials and residing on rough surfaces of the pore space.
Figure 12 shows 2D slices from 3D MR images after
imbibition for 8 seconds with average water saturation of
26.3%. The water progressed towards, but had not yet
reached the center of the sample in these images. A uniform
water saturation distribution behind the waterfront is ob-
served. The DDIF and Conical-SPRITE experiments were
reproducible after a time interval of 15 minutes. Therefore
the changes in water distribution in the core do not occur
once the core is moved from the water reservoir.
Figure 13 shows 2D slices from a 3D MRI data set after
imbibition for 15 seconds with an average water saturation of
30.9%. The penetrating waterfronts have just merged at the
center of the sample. The images reveal a uniform water
distribution.
Figure 14 shows 2D slices from a 3D MRI data set after
imbibition for 3 minutes and 53 minutes with average water
saturation of 45.6% and 51.5%. The two images show a ho-
mogeneous distribution with a uniform increase of water
saturation.
The MRI results indicate that water saturation increases
globally once the penetrating waterfronts have merged.
These results are consistent with a lm type penetration
mechanism with a subsequent lling of larger diameter pores
as suggested by the DDIF experiments.
There are two main mechanisms for water saturation
evolution, i.e., a water-lm front advance mechanism and
water-lm thickening mechanism. Before waterfronts reach
the center part of the sample, water ows along the corner
and surfaces of the pore network, while air ows along the
center of the pore space. After the waterfronts meet and
merge at the center part of the sample, water ows continu-
ously with a lm-type mechanism, making the pre-existing
water-lm thicker. This results in a more uniform water dis-
tribution with an increase of water saturation during counter-
current imbibition.
During counter-current imbibition, the wetting phase
water and nonwetting phase air ow in the same pore-
throat channels with opposite direction, resulting in an extra
viscous resistance and reduced cross-sectional ow area of
each phase for counter-current imbibition compared with co-
current imbibition. This is especially true in the case of water
and oil, which is the reason that counter-current imbibition
has a lower imbibition rate, and lower displacement ef-
ciency, under similar boundary conditions.
27
FIG. 11. The DDIF spectra during counter-current imbibition acquired at
different water saturation Sw levels. The area under each curve is propor-
tional to the water saturation. After imbibition for 8 seconds, the overall
water saturation was 26.3%. The DDIF spectrum shows a very low satura-
tion in pores and relatively higher water saturation in throats. After imbibi-
tion for 84 minutes, the overall water saturation was 56.0%. The water
saturation did not signicantly increase with further imbibition.
FIG. 12. 2D slices from a 3D Conical-SPRITE MRI data set of partially
saturated Berea sandstone core. Longitudinal a and transverse b slices are
displayed after the core was immersed in the water for 8 seconds. The
overall water saturation was 26.3%. The penetrating waterfronts have not
yet reached the sample center. The FOV was 7 cm7 cm, and slice thick-
ness was 1 mm.
FIG. 13. 2D slices from a 3D Conical-SPRITE MRI data set of partially
saturated Berea sandstone core. Longitudinal a and transverse b slices are
displayed. After 15 seconds of counter-current imbibition, the overall water
saturation was 30.9%. The penetrating waterfronts have just merged, and a
uniform water distribution is observed in the images. The FOV was 7 cm7
cm, and slice thickness was 1 mm.
FIG. 14. 2D longitudinal slices from a 3D Conical-SPRITE MRI data set of
partially saturated Berea sandstone core. a After counter-current imbibition
for 3 minutes with overall water saturation was 45.6%. b After counter-
current imbibition for 53 minutes with overall water saturation of 51.5%.
The images show uniform water distribution. The FOV was 7 cm7 cm,
and slice thickness was 1 mm.
9615 J. Chem. Phys., Vol. 119, No. 18, 8 November 2003 Pore lling processes
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CONCLUSIONS
During spontaneous co-current imbibition, water dis-
places air through the pores and throats uniformly with a
piston-like pattern. An approximately constant water satura-
tion distribution is observed behind the advancing water-
front.
During counter-current imbibition, water ows through
the pores and the connected throats with a lm-type struc-
ture, along the corners and the surfaces of the pore space,
while air ows along the center of pores and throats in the
opposite direction. After the penetrating waterfronts meet at
the center part of the core, the pre-existing water lm thick-
ens, resulting in a global and uniform increase in water satu-
ration.
This study has for the rst time combined the DDIF pore
size distribution method in partially saturated porous media
with Conical-SPRITE MRI. Each technique has great poten-
tial for the study of multi-phase uid ow in porous media.
ACKNOWLEDGMENTS
This work was supported by equipment and operating
grants awarded to B.J.B. by NSERC of Canada, as well as an
Atlantic Innovation Fund award to MKG. B.J.B. thanks the
Canada Chairs Program for a Research Chair in MRI of ma-
terials. We would also like to thank Dr. Bryce MacMillan,
Rod MacGregor, and Meghan Halse for their help with vari-
ous aspects of the experiments.
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