|
|
Residual fluid dissolution fingering in porous media:
Experiment in a water-air system
FRITZ STAUFFER, OSCAR OSORIO and WOLFGANG
KINZELBACH
Institut für Hydromechanik und Wasserwirtschaft
Eidgenössische Technische Hochschule Zürich,
CH-8093 Zürich, Switzerland
Ph.: +41-1-633 30 79; Fax: +41-1-633 10 61;
email: stauffer@ihw.baum.ethz.ch
ABSTRACT
The dissolution of immiscible fluid entrapped at
residual saturation in porous media by flushing is investigated for the case of
a water-air system, which represents an analogy to the dissolution of residual
NAPLs in groundwater. A quasi-saturated sand packing at residual air saturation
was horizontally flushed with deaerated water. Visible dissolution fronts could
be discerned at the tank walls and their evolution was recorded. The
dissolution fronts soon showed distinct fingers that increased in length from
zero up to 19 cm over a total horizontal flow distance of 70 cm. These fingers
were similar to the dissolution fingers described by Imhoff et al. (1996) for residual
NAPLs. Tracer tests without dissolution effects were performed on the sand
packing at residual air saturation. They showed that the packing was slightly
horizontally layered and that the positions of the dissolution fingers in the
sand packing coincided with zones of higher velocity. However the length of the
dissolution fingers was more than two times larger than the length of the
corresponding tracer fingers. Although similar results can be expected for the
dissolution of residual NAPLs in groundwater, their applicability has to be
further verified.
Keywords: Groundwater, residual air saturation,
dissolution, hydraulic conductivity, inhomogeneity, fingering, analogy to
NAPL-water systems
INTRODUCTION
Many groundwater contamination problems are caused by
a release of immiscible liquids (Non Aqueous Phase Liquids, or NAPLs) into the
subsurface, e. g., by a discharge of chlorinated hydrocarbons. The NAPL first
migrates through the unsaturated zone until it reaches the saturated zone.
After the bulk of the NAPL has migrated through the subsurface, a substantial
fraction will remain trapped in pores. In saturated groundwater systems, these
liquids are subject to a series of physical mechanisms. An important part of
them remains immobile in the porous medium at a residual saturation, forming a
source of long-term contamination of the groundwater caused by the low
dissolution rate. The rate and manner in which a NAPL dissolves in groundwater
will determine the magnitude and duration of contamination. A good
understanding of the dissolution process contributes to the evaluation and
optimisation of remediation measures.
Several theoretical and experimental studies have been
performed on the dissolution of trapped fluids in porous media (e. g., Powers
et al., 1994; Imhoff et al., 1994). In previous experiments (Imhoff et al.,
1996), it was observed that the dissolution of residual NAPLs leads to
instabilities causing fingers in the moving dissolution front.
This study is conceived as an experimental investigation
of the dissolution of residual air in a quasi-saturated sand packing by
flushing. The main focus is on the detection of the temporal evolution of the
visible dissolution front. The experiment is an analogy to the dissolution of
residual NAPLs in groundwater and is much more conveniently performed than a
corresponding experiment with NAPLs.
EXPERIMENTAL SET-UP
The experiment was conducted in a Plexiglas tank with
inside dimensions of 78 cm in horizontal length, 30 cm in vertical height and 8
cm in width. The tank was subdivided into three domains, an inlet reservoir, a
69.4 cm long porous packing, and an outlet reservoir. The packing was confined
by two perforated vertical aluminium walls with a sandwiched polyamid web. A
pump was placed between a storage tank for deaerated water and the inflow
reservoir. The outlet reservoir was connected to a constant head vessel.
Therefore a horizontal flow could be established in the porous packing. The
sand used for the packing was a medium uniform quartz sand of the grain size
0.5-0.75 mm.
EXPERIMENTAL METHOD
The sand was packed by using a falling strands method.
The method consisted of letting dry sand fall through a 4 cm diameter tube with
a length of 51 cm, equipped with three sieves at the bottom. The instrument was
slowly moved horizontally during the packing procedure. The method may cause a
slight horizontal layering of the sand packing. The sand packing had an average
height of 27.1 cm.
The dry sand packing was slowly flushed with tap water
at room temperature until quasi-saturation was obtained, the trapped air
remaining in the medium. The water weight in the tank was measured and the
residual air saturation determined. Water was deaerated during 10 min in a 2.5
l volume container using a vacuum pump and then pumped to the storage tank. At
the beginning of the experiment the volume of water in the space between the
inlet and the sand packing was replaced by deaerated water. The sand packing
was horizontally flushed with deaerated water at a rate of 87 ml/min. Periodic
measurements of the inlet and outlet water levels as well as of the outflow
were performed in order to determine the temporal development of the hydraulic
conductivity. The advance of the dissolution front was optically observed at
the tank walls by means of an illumination that facilitated the visualisation
of the air bubbles zone.
Two tracer tests without air dissolution were
performed on the quasi-saturated sand packing. A solution of 100 ppm Eosin dye
solution without deaeration was used as tracer and introduced into the system
as a long pulse input (tracer breakthrough {test I} and subsequent flushing
with tap water {test II}) at the same flow rate as the deaerated water in the
dissolution experiment. The visible tracer fronts were periodically observed
and registered on both sides of the tank.
RESULTS AND DISCUSSION
The measured and calculated hydraulic parameters of
the experiments are listed in table 1. The sand packing was flushed with 39
pore volumes (PV) of deaerated water. It was observed that air bubbles
continuously shrank due to dissolution, until they disappeared within a zone of
less than 1 cm of length. Figure 1 shows the temporal development of the
dissolution front, with the inlet at x = 0, and the outlet at x = 69.4 cm.
After the packing was flushed with about 2 PV of water (t = 135 min), a clear
dissolution front with a rather uniform pattern was visible. However, at the
points y = -10 cm, +2 cm and +8 cm the dissolution was more rapid than in the
rest of the front. After 4 PV of water (t = 270 min), small fingers clearly
developed with lengths between 1 and 3 cm. The finger length increased rapidly
as the flux of water continued. After 39 PV of water (t = 2485 min), the length
of the fingers ranged between 9 and 19 cm. The comparison between the left and
right tank sides shows that the general structure was rather similar. Five main
peaks were discerned on both sides. A measure of the finger length lf
can be defined as half the distance between the peak x-position minus the
x-position of the next depression above. The development of lf over
time is shown in figure 2. The growth of most fingers was approximately
proportional to time. The mean thickness of all fingers remained almost
constant during the experiment (between 1 and 4 cm). The thickness to length
ratio of the fingers remained at about 1 to 5. The mean front velocity was
found to be 3.3×10-4
cm/sec and was almost constant. The front on the right side of the tank was
slightly slower than on the left side. The final mean hydraulic conductivity
was nearly doubled due to the dissolution of the entrapped air.
|
Porosity n |
0.35 |
|
Residual
air saturation Sa |
0.08 |
|
Hydraulic
conductivity K(1-Sa) from dissolution experiment Hydraulic
conductivity K(1-Sa) from tracer experiment |
0.11 cm/s 0.13 cm/s |
|
Saturated
hydraulic conductivity Ksat |
0.19 cm/s |
Table 1 Hydraulic parameters
of the sand packing

Fig. 1 Evolution of the
dissolution front with fingers, inflow at x = 0
|
|
|
Fig. 2 Dissolution finger length
over time
The two tracer tests showed that the location of the
visible tracer fingers were essentially identical and thus the tests were fully
reproducible. It can be concluded that the visible tracer fronts approximately
coincide with the advective tracer fronts disregarding molecular diffusion and
dispersion effects. The resulting mean tracer velocity was 0.017 cm/sec. Figure
3 shows the displacement of the tracer front through the sand packing for test
I. From x = 0 to x = 5 cm the tracer front points (along the y-axis) moved at
almost the same velocity. At front position 3 at x=22.5 cm, three zones were
visible which could be interpreted as small fingers. Fronts on both sides of
the tank were again similar. They indicate a slight horizontal layering of the
sand packing resulting mainly in a vertical variability of the velocity
vectors. Again five major peaks can be discerned at later times. The positions
of these fingers along the y-axis coincided with those of the dissolution
fingers but the shape of the fingers was not identical. The development of most
tracer finger length was again approximately proportional to time (Fig. 4).
This indicates that the visible tracer fingers were essentially advection
dominated.

Fig. 3 Evolution of the tracer
front, inflow at x = 0
|
|
|
Fig. 4 Tracer finger length over
time
The length of the dissolution fingers was 2.2 to 3.8
times larger than that of the tracer fingers. The finger development can be
explained as follows. In a layered sand packing the initial specific flux is
proportional to the initial hydraulic conductivity of a considered layer. This
leads to an increased flux in high-conductivity layers coupled with an
increased dissolution capacity compared to the mean flux. Therefore a finger
development is expected in high-conductivity layers. The porous medium is fully
saturated behind the dissolution front. Therefore the hydraulic conductivity is
about doubled in finger regions. As a consequence the water flux in a finger is
further increased resulting in a rapid growth of the finger length.
For the dissolution of residual NAPLs in groundwater
similar results can be expected. This is supported by the fact that essential
parameters controlling the interphase mass transfer are the residual fluid
saturation and the free liquid diffusion coefficient (Imhoff et al., 1994)
which are in a similar range for air-water systems. However the applicability
to NAPLs has to be further verified by taking into account entrapment,
mobility, dissolution characteristics, and residual saturation of the fluid
under consideration.
CONCLUSIONS
The dissolution of immiscible fluid entrapped at
residual saturation in porous media was investigated for a water-air system.
The dissolution of residual air caused by flushing a quasi-saturated sand
packing with deaerated water showed a clearly visible moving front with fingers
which increased in length from zero to 19 cm over a flow distance of 70 cm.
These fingers were similar to the dissolution fingers described by Imhoff et
al. (1996) for the dissolution of NAPLs. The fingers grew approximately in step
with the mean front displacement. With the help of tracer tests it was
demonstrated that the sand packing was slightly horizontally layered and that
the position of the dissolution fingers coincided with zones of higher
velocity. The length of the dissolution fingers was more than two times larger
than the length of the corresponding tracer fingers. It can be stated that the
dissolution process amplifies the relatively small contrast in hydraulic
conductivity in the front region. The experiment indicates that macroscopic
variability in hydraulic conductivity may control finger location and growth
and thus the dissolution efficiency. Similar effects can be expected for the
dissolution of residual NAPLs in groundwater.
ACKNOWLEDGEMENTS
The
second author acknowledges the grant he received from the Swiss Confederation.
REFERENCES
Imhoff,
P. T., P. R. Jaffé, and G. F. Pinder, An experimental study of complete
dissolution of an non aqueous phase liquid in saturated porous media. Water
Resour. Res., 30 (2), 307-320, 1994.
Imhoff
P. T., G. P. Thyrum, and C. T. Miller. Dissolution fingering during the
solubilization of nonaqueous phase liquids in saturated porous media 2.
Experimental observations. Water Resour. Res., 21 (7) 1929-1942, 1996.
Powers,
S. E., L. M. Abriola, and W. J. Weber, An experimental investigation of
nonaqueous phase liquid dissolution in saturated subsurface systems: Transient
mass transfer rates. Water Resour. Res., 30 (2), 321-332, 1994.