Chemhd&&eering Science. Vol. 41, No. 2, pp. 273-281, 1986 uax-2so!wt6 53.00+0.

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Printed in Great Britain. Pergamoa Pmss Ltd.

A FILTRATION MODEL FOR THE FLOW OF DILUTE,

STABLE EMULSIONS IN POROUS MEDIA-II. PARAMETER
EVALUATION AND ESTIMATION

H. SOO, M. C. WILLIAMS and C. J. RADKEt

Chemical Engineering Department, University of California, Berkeley, CA 94720, U.S.A.

(Received 25 June 1984)

Abstract-Part I of this work outlined a new theory, based on deep-bed tiltration concepts, to describe the
flow of dilute, stable emulsions in underground porous media. Here, in Part II, we quantitatively test the
proposed theory against experimental data and we indicate how the liltration model parameters can be
estimated from first principles.
Comparison is made between the theory and data on transient permeability and efauent concentration for
dilute, oil-in-water emulsions of mean drop-size diameters ranging from 1 to IO- and volume
concentrations of 0.5-2.5 /, flowing in quartx sandpacks of 0.57-2.0 & permeability. The pH of the
continuous aqueous phase is kept constant at 10. Filtration theory successfully represents the data, permitting
unambiguous evaluation of the theoretical parameters
Procedures are described for o priori calculation of the filtration parameters from knowledge of the drop
sixe and the pore-size and grain-sixe distributions of the porous medium. God agreement is achieved between
the experimentally determined parameters and their estimated values. Thus, the proposed filtration model
provides a reliable tool for predicting emulsion flow behaviour in porous media

lNTRODUCTION sion flow models (McAuliffe, 1973; Devereux, 1974a)

Available experimental evidence indicates that stable
emulsions percolate through underground porous
media by capture of the disperse phase with sub-
sequent permeability reduction to the continuous
phase (McAuliffe, 1973; Devereux, 197423; Alvarado
and Marsden, 1979; Soo and Radke, 1984). While
flowing in the porous medium, droplets clog pores
having sixes smaller than their own by lodging between
sand grains (straining capture). Also, they are trapped
in recirculation eddies, wedge in the crevices, or
sometimes attach to the pore walls due to van der
Waals, electrical, gravitational and hydrodynamic
forces (interception capture). As drop retention builds,
the permeability of the medium is reduced and 3ow
diverts to the larger pores where capture probability is
lowered because of the increasing pore sixes.
In Part I of this series we presented a filtration-based
flow model which correctly accounts for the actual
physical phenomena occurring in the porous medium.
In that theory, transient flow behaviour is character-
ized by three parameters: a filter coefficient, a dow-
diversion parameter and a flow-restriction parameter.
The filter coefficient controls the sharpness of the
emulsion front, the flow-diversion parameter dictates
the steady-state retention as well as the flow-
redistribution phenomenon, and the flow-restriction
parameter describes the effectiveness of retained drops
in reducing permeability. Qualitative comparison of
the filtration theory to the continuum-viscous
(Alvarado and Marsden, 1979) and retardation emul-
%%zsent address: Union Carbide Corporation, South
Charleston,WV 25303, U.S.A.
*To whom correspondence should be addressed.
273
revealed the critical import of testing model predic-
tions against effluent drop concentrations in addition
to validating flow resistance_
In this second part we bring theory and experiment
together. The filter coefficient and the flow-diversion
parameter, which both control the processes of drop
capture in the medium, are evaluated from emulsion-
concentration histories. Conversely, the flow-restric-
tion parameter, which characterizes how effective
retained drops are in obstructing flow, is obtained
from permeability data. Quantitative comparison is
made between the theory and the experimental results
for dilute, oil-in-water emulsions of mean drop di-
ameters ranging from 1 to 10 pm and volume con-
centrations of 0.5-2.5 okflowing in quartz sandpacks of
0.57-2-O pm* permeability. The proposed filtration
model successfully represents the experimental data,
both for permeability-reduction and dropcon-
centration histories.
Since the three filtration parameters have well-
defined meanings, we develop simpli6ed procedures
for their estimation from physical properties of the
system, such as the medium porosity, the pore-size and
grain-size distributions, and the drop size. The
periodic-constricted-tube model is adopted to describe
the porous medium (Payatakes et al., 1973).
Accordingly, the filter coefRcient is estimated based on
the likely capture probability of drops in a unit bed
element (Payatakes et al., 1974). The flow-
redistribution parameter is estimated from fractional
monolayer coverages of drops on grain surfaces and
from the deduced volume fraction of blocked pores.
Finally, the flow-restriction parameter is estimated
from hydrodynamic calculations of the increased
274
pressure drop due to retained drops in a constricted
tube.
In the next section we deal with the evaluation of
the filtration parameters from experimental data. This
is followed by a discussion of parameter estimation
procedures.
PARAMETER EVALUATION
Experimental
Only a brief account of the experimental procedures
is presented here. Considerable detail may be found
elsewhere (Soo, 1983; Soo and Radke, 1984). Dilute,
oil-in-water emulsions of mean drop sizes (D, >
ranging from 1 to IO pm and of known drop-size
distributions were injected into quartz sandpacks of
known grain-size distribution, pore-size distribution
and initial permeability KO. Drop-volume concentra-
tions ci of 0.5, 0.6, 1.2 and 2.5 y0 were used, and the
superficial velocity u was fixed at 0.07 mm/s. The
emulsion droplets were adjusted to neutral buoyancy
with carbon tetrachloride. A dilute aqueous sodium
oleate-oleic acid mixture at a pH of 10 stabilized the
emulsion. Under this alkaline condition there is signifi-
cant double-layer repulsion between the oil drops and
between the drops and the quartz sand grains.
Sensitive transducers (Validyne) monitored the pres-
sure drop. To permit flow-model discrimination, the
core effluent was sampled periodically and analysed
(Zeiss Particle Counter) for drop concentration and
size distribution.
Filtration theory
According to the filtration flow theory proposed in
Part I, the transient drop-volume retention and drop-
volume concentration profiles c (t, JC)and c (t, x) obey
the following expressions in a linear medium of length
L:
1 -exp (aA,,c,T)
c(T,Z)
____%I = a [l -exp (A,%) -exp (ahs,ciT)]
c(T, 3)
-=- Q cc 2)
ci uiG7
where f = x/L is a reduced axial distance, and T =
z --f is a shifted time variable with 7 = ut/EOL. The
subscript i refers to the bed inlet and E,,is the clean-bed
porosity. As, = &,L is the reduced filter coefficient,
made dimensionless by the column length L, while a is
the flow-redistribution parameter.
Emulsion flow behaviour is reflected in the transient
permeability reduction, K/K,,. According to Part I,
this ratio depends on the local retention as
1 TCi*
-= [ 1 - #?a/~~] - 1 dn,
where fi is the flow-restriction parameter.
From eqs (1) and (2), the filtration parameters A,,
and a are seen to control droplet chromatography (see
also Figs 3 and 4 of Part I). Therefore, they are best
H. Soo er al.
evaluated from experimental effluent-concentration
histories, cL = c(T, 1). In contrast, fi influences flow
resistance (see Fig. 5 of Part I), and is, therefore, best
evaluated from experimental pressure-drop data.
Details of how the filtration parameters are actually
fit from the experimental results may bc found in
Appendix A.
Comparison to experiment
Figure 1 compares typical experimental flow data to
the filtration theory. The transient reduced overall
permeability K/K0 and the reduced effluent drop-
volume concentration cL/ci are plotted against the
cumulative injected volume of oil, TC~_Solid symbols
correspond to transient permeability reductions and
open symbols correspond to effluent emulsion concen-
trations. Dashed lines show the best fit of the theory to
the effluent concentrations according to eqs (1) and (2),
as described in Appendix A. Likewise, the solid lines
are best-fit transient permeabilities according to eq. (3).
Figure 1 demonstrates that the proposed filtration
theory successfully portrays both the transient per-
meabilities and the drop breakthrough concentrations,
even with the assumption that model parameters a and
B are retention-independent. Additional confirmatory
flow data are reported in Figs 6 through 12 of Soo and
Radke (1984), where in those figures the solid and
dashed lines are best fit according to the filtration
theory. Table 1 summarizes the filtration model par-
ameters obtained in this work.
In Fig. 1, K. = 1.15 pm2 and the inlet mean drop
sizes vary from 2.1 to 6.1 pm. As the drop sizes increase,
the effluent concentration curves reveal that drop
retention increases so that 1/a rises (i.e. the steady-state
retention is an increasing function of drop size).
Permeability at any 7ci decreases as the mean drop size
increases from 2.1 to 4.5 pm. Yet, initially, the rate of
permeability reduction is smaller when the drops
(1) increase in size from 4.5 to 6.1 pm. This is @cause fl is a
decreasing function of drop size, due to its unit volume
definition, as verified in Table 1. At equal volumes of
<OdhF" 1
Ci=OOOS _
PORE VOLUME OIL
(3)
Fig. 1. Experimental permeability-reduction (solid symbols)
and breakthrough-concentration (open symbols) histories for
varying drop sizes (2.1, 3.1, 4.5 and 6.1 Nrn) in the 1.15 pm2
permeability core. The oil viscosity is 1.5 mPa s. Solid (per-
meability reduction) and dashed lines (breakthrough-
concentration) are best _.fit according to _.
the filtration theory
. . -_. _
with the correspondmg parameters hsted m .laOle 1.
 Filtration model for the flow of dilute, stable emulsionsin porous media-11 275

Table 1. Filtration parameters

2.5 0.57 0.038 15.0 4.7 0.570

3.3 0.57 0.045 14.5 4.4 0.563
3.6 0.57 0.047 14.5 1.6 0.682
5.3 0.57 0.250 3.6 - 0.900
2.1 1.15 0.019 13.9 0.69 0.264
3.1 1.15 0.032 14.5 1.7 0.464
3.7 1.15 0.027 12.6 1.8 0.340
3.8 1.15 0.032 7.9 2.4 0.253
4.3 1.15 0.051 14.0 3.5 0.714
4.4 1.15 11.7 1.5 0.702
4.5 1.15 :z 10.0 1.9 0.530
4.5 1.15 0.074 10.2 1.9 0.755
5.8 1.15 0.095 5.9 1.7 0.561
6.1 1.15 0.170 4.8 1.4 0.816
6.4 1.15 0.200 3.6 2.8 0.720

retained oil, smaller drops are more finely dispersed

locally in the pore assemblages, and are therefore more
effective in reducing permeability. Hence, before drop-
let breakthrough where retention volumes are equal,
the 4.5 m drop emulsion has a lower transient c;
permeability than the 6.1 pm drop emulsion. A 0.006
0 0.012
Eventually, at steady state, large drop-size emulsions 0 0.025
reduce permeability more than small drop-size emul-
sions. That is, in a given porous medium, p/a is an
increasing function of drop size (i.e. at steady state
K-/K,, = 1 -/?/a). Table 1 also confirms this observa- ol; 0 I I I
0
tion, with some scatter. 0.05
c, (T-1)
0.10 0.15

One unique characteristic of the filtration model is

that both effluent concentrations and transient per- Fig. 2. Experimental breakthrough-concentration histories
meabilities should be independent of the disperse oil- for varying injection concentrations (0.6, 1.2 and 2.5 vol %) in
phase viscosity. Figure 11 of Soo and Radke (1984) the 2 pm permeability core. The oil viscosity is 1.5 mPa s
while the dashed line is best fit from the 0.6 and 1.2 vol /,
shows that upon changing the oil viscosity from 1.5 to concentration data according to the filtration theory
23 mPa s, while keeping all other variables constant, (l/a = 0.015, fi = 15 and AsI = 1.6cm-I).
no change in transient permeability or emulsion-
concentration history is observed. This provides con-
vincing evidence that the filtration model correctly I
I I I
1
reflects the phenomena controlling dilute, stable emul-
sion flow in unconsolidated porous media.
A second distinguishing feature of the filtration
model in eqs (l)-(3) is that graphs of cL/ci and K/K, vs.
the variable ci (7 - 1) should be independent of inlet
concentration. Figures 2 and 3 give results for injecting
a 4 m mean drop-size emulsion of ci = 0.006, 0.012
and 0.025 volume concentrations into a 2 pm2 per-
meability sandpack. Both cL/ci (Fig. 2) and K/K,
(Fig. 3) obey the filtration theory for the two most
dilute suspensions. Deviations toward higher retention ci (T- I)
and larger permeability reduction are found with the ci
= 0.025 emulsion. Such deviations may be attributed Fig. 3. Experimental permeability-reduction histories for
to larger hydrodynamic resistances (e.g. ~JF, > 1) or varying injection concentrations (0.6,1.2 and 2.5 vol %) in the
2 pm* permeability core. The oil viscosity is 1.5 mPa s while
to a nonlinear dependence of drop capture kinetics on the solid line is best fit from the 0.6 and 1.2 vol y0
concentration in eq. (4) of Part I. concentration data according to the filtration theory (l/a
The delayed effluentconcentration history of the = 0.015, /I = 15 and AsI = 1.6cm-).
0.025concentration emulsion in Fig. 2 suggests non-
linear kinetics as the cause of the discrepancy. There solid particulates (Herzig et al., 1970). The present
are citations in many deep-bed filtration studies that ci study indicates linearity prevails for liquid droplets up
= 0.001 is the upper limit of linear capture kinetics for until about ci = 0.01. Drop capture kinetics are in-
276 H. so0 et al.
fluenced by interactions among the drops. In par-
ticular, high drop concentrations can lead to several
drops being captured simultaneously in a pore, which
at low drop concentration does not plug. The dashed
line in Fig. 2 and the solid line in Fig. 3 represent the
best-fit calculations of the two lower concentration
experiments according to eqs (lF(3). Thus, the fil-
tration model successfully interprets the experimental
results up to about ct z 0.01.
We conclude that the transient filtration model
accounts for all the experimental findings for emulsion
flow cited in Part I. Furthermore, it quantitatively fits
pressure drop-flow rate data and e5uent drop concen-
trations with a single set of parameters.
PARAMETER ESTIMATION
Prediction offiltration parameters
The phenomenological filtration parameters A,,, a,
and /l all have well-defined physical meanings. From
the theoretical analysis of Part I the expressions for
these parameters are [see eqs (lo), (11) and (13) of
Part I]:
and
XdD,
J, (5)
The symbols appearing in eqs (4)-(6) are defined in
Part I. In this study the surface properties of the drops
and the sand grains are Iixed. Therefore, eqs (4)-(6)
permit calculation of I,,, a and /l given fundamental
information about the drop size and pore-size distri-
bution along with some estimates of the porous-
medium structure (& D,, up,_,), of the interception
capture probability (A,,), and of the retention hydro-
dynamic resistance (/$,). In the following sections we
develop procedures for predicting the filtration para-
meters. The experimentally determined values listed in
Table 1 are then compared to the a priori predicted
ones.
Filter coeficient
Overall drop capture efficiency, or the filter coef-
ficient, may be estimated from eq. (4):
ils, = < 11,> (as/so) + <A, > (1 -es/so), (7)
where < L, > and <AI > are the porosity-averaged filter
coefficients in the pores where straining occurs (D,
c DJ and where interception occurs (D, > D,),
respectively. First, we define the porosity of the
straining pores, es, in terms of the transition pore-
throat diameter between straining and interception
pores, D,, so that
et E,,dD,.
(8)
Es =
I0
As indicated later, stabilized liquid drops are not
captured on top of previously retained droplets.
Hence, the constricted-tube transition diameter should
lie, from simple geometric arguments, between 2 and 3
drop diameters. From our experimental results for a
and /I, we will show D, to be close to 2 <D,>.
The straining porosity, ss, may now be calculated,
since the pore-entry diameter distributions of the
sandpacks are known from centrifugal water-drainage
experiments (Soo, 1983). These experiments show that
the volume frequency of pore throats (i.e. E,,/E~) is
distributed according to log-normal statistics. Hence,
es follows directly:
exp ( - 5/2) dth (9)
where In ii and 6 are, respectively, the mean and the
standard deviation of the Gaussian distribution in
In D, which serves as the generating function for the
log-normal distribution (Thomasian, 1967). Once ii
and 6 .are obtained from experiments and D, is
specified, eq. (9) dictates the value of ES.Further, eq. (9)
states that es. and consequently A,,, are functions of
[In (0,/p)]/& the dimensionless transition throat dia-
meter based on a log-normal pore-sire distribution. It
remains to determine < 1, > and < 1, >.
As discussed previously in Part I, drop capture
efficiencies, q,,, in the straining pores are close to unity.
Therefore, < 1, > may be approximated by the inverse
of the thickness of the average unit bed element,
1E agsrl, dD,. According to Payatakes et al. (1973), 1
50
is related to the physical properties of the unconsoli-
dated porous medium by
1
-yl= &,) <D:>]l (12
2
<s>
where D, is the grain diameter and ( Di>
= wfgD;dD,, where fg is the volume grain-size
s
distkbution. We find ( D3 > and hence < As > from sieve
analysis of the sand grails (Soo, 1983).
Next, <A, > in the interception pores, where only
surface capture occurs, can be estimated from trajec-
tory calculations of a particle moving through a
constricted tube, or around a cylindrical or spherical
collector (Tien and Payatakes, 1979). The calculation
for a constricted tube, including all possible physical
forces, follows from the work of Payatakes et al.
(1974). For a mean drop-size to pore-size ratio between
0.01 and 0.1 (i.e. in the interception pores), the capture
efficiency with no net colloidal interaction forces
ranges from 1O- 3 to 1O- [see Fig. 2 of Payatakes et al.
(1974)]. Thus, within the unit-bed-element model we
take (I, > to be equal or less than about 0.01 /L This
completes the estimation of parameters needed to
calculate A,, from eq. (7).
Figure 4 demonstrates the relation between
(&J)- and the dimensionless transition diameter
[In (D,/p)]/S for two values of <I, >. Here D, is taken
 Filtrationmodel for the flow of dilute, stable emulsionsin porous media-11
- KoomJ=) o most pronounced for the larger drops in Fig. 4, since
,*I- 0 1.15
l 0.57
Dt - 2<Dcl>
lo I
-3.0 -2.0
I t
-10
[In (Dt/&i )I /8
Fig. 4. The inverse of filter coefficient, expressed as &I,
correlatedagainst the dimensionless logarithmic transition
pore-throat diameter [In (D,/ji)]/6. D, is taken as 2 <Dd > in
this figure.
as 2 <Dd>. The physical meaning of (&I)- is the
number of unit bed elements (i.e. the number of grain
diameters) a drop travels before it is captured. Open
circles in the figure represent experimental results of a
1.15 m2 permeability sandpack and solid circles rep-
resent those of a 0.57 pm2 permeability sandpack.
Selected error bars denote the expected variation of the
experimental values. The log-normal distribution par-
ameters, reported in terms of R and 6, are obtained
from centrifuge water-drainage measurements (Soo,
1983). For the 1.15 pm2 sandpack, R is measured as
25.5 pm and 6 is 0.54 (i.e. <D,> = 29.5 pm+). For the
0.57 m2 sandpack, ji is 15.3 pm and 6 is 0.49 (i.e.
<Dp > = 17.3 m). The unit-bed-element length, 1, is
calculated from eq. (10). For the 1.15 pm2 sandpack it
is 120 pm (i.e. a mean grain diameter of 107 pm), and
for the 0.57 pm2 sandpack it is 83 pm (i.e. a mean grain
diameter of 75 pm).
At small values of the logarithmic-reduced trans-
ition diameter, or equivalently for small mean drop
sixes, the drops travel many tens of unit bed elements
before they are captured. As the mean drop size
increases, the drops travel a fewer number of unit bed
elements before they stick.
Solid lines in Fig. 4 represent a priori predictions
based on eqs (7~(10) for <A,> equal to lo-/1 and
lo- j/l. At large values of the logarithmic-reduced
transition diameter, the prediction shows that strain-
ing capture dominates. Most drops are retained
within one unit-bed-element distance, and therefore
(&tW approaches unity. At small values of
[ln (D,/R)]/S, (1,,Z)- approaches (<A,> I)- . Signili-
cant deviations are seen for the larger drops
independent of < 1, >. This may be explained qualitat-
ively by the drop-size separation effect reported by Soo
and Radke (1984). In emulsions with a drop-size
tFrom the definitionof the log-normal distributionfunc-
tion, the mean-volume Pore-throat diameter is given by:
(D, > = ji [exp (S2/2)] (Thomasian, 1967; Soo, i983).
277
distribution, the small drops percolate through the
porous medium more quickly than the large ones. The
spread of the experimentally measured breakthrough
curve, which determines IsI, therefore is wider than
that of a monodisperse system with the same mean
drop size. A wider effluent drop-concentration spread
is interpreted by the theory as a smaller or under-
estimated A,,. This size-separation phenomenon is
the emulsions with a large average drop size possess a
wider distribution (Soo and Radke, 1984). Fortunately,
when 1,, is large, it has little influence on the emulsion
flow behaviour (see Fig. 3 of Part I).
Flow-diversion parameter
An estimate of CL,the flow-diversion parameter, is
available from eq. (5). At steady state, the retention in
each classification of pore space is at a fixed value so
that cp - ss for D, -z D, and up - ur,,, for D, > D,.
Under this circumstance, eqs (4) and (5) reduce to:
a m= s0/gm = so/(es+ <o,,,>) 9 (11)
where < ur,m> is the average maximum retention in the
interception pore space and ss is available from eq. (8).
In this study drops are not captured on previously
retained drops. Hence, the maximum interception
retention is that of complete monolayer cover-
age or oI.m = [2x(1 -so) (so --ES) <D,>ll(fi <D,>)
(Payatakes et al., 1973).
In reality, however, complete surface monolayer
coverage is highly unlikely, especially for large drops
and for repulsive double-layer interactions. Therefore,
a fractional coverage, 8, is introduced:
2n-50(1 -so) (1 - E~/EO)<D, > e
<QI,m> = fQ,,@ =
,b<D,> .
(12)
Equations (9), (11) and (12) permit calculation of am,
which we take as a good approximation to a based on
the results of Fig. 2 of Part I.
Figure 5 displays the functionality of l/a with the
dimensionless logarithmic-transition pore-throat di-
ameter [ln (D&i)]/& Circles give the experimental
data for the two different permeability cores. This
figure demonstrates that as drop size increases, l/a
increases. As drop size increases,. more drops are
captured in the porous medium. Consequently, flow
redistribution is more manifest, and steady-state reten-
tion is higher.
Solid lines in the plot represent the a priori calcu-
lations of a for various values of interception coverage
8 and for D, fixed at 2 <D, >. It is not possible to obtain
a unique estimate of 8 and D, using only data in Fig. 5.
Raising D, simply lowers 0 because a larger D, de-
signates more retention in the straining mode and
therefore less retention in the interception mode. Thus,
the dashed line in Fig. 5 for D, = 2.2 < Dd > and 0 = 0.1
lies above the solid line for D, = 2.0 < D, > and 0 = 0.1.
To obtain 8 and D,, we utilize both the data for a in
Fig. 5 and the data for fi in Fig. 6 (to be presented).
278 H. Soo et nl.
-3.0 -2.0 -1.0
ClnK+/p)l/s
Fig. 5. The inverse of the flow-diversion parameter, 01,
correlated against the dimensionless logarithmic transition
pore-throat diameter [ln(D,/@)]/& B is the fractional grain
surface coverage of drops captured in the interception mode.
Two estimates of Dt are reported (solid and dashed lines).
20 I I I I
2 0, e = 04 1 For stable emulsion flow in porous media, however,
9%2=
0 I L I
-3.0 -1.0
b n Cf$%],s
Fig. 6. The flow-restriction parameter j3 correlated against
the dimensionless logarithmic transition pore-throat dia-
meter, [ln (Dt /F)] /6. Solid and long dashed lines correspond
to <fit > = 18 while the short dashed line corresponds to
<#?t> = 20. e is the fractional coverage of grain surfaces
occupied by drops retained due to interception.
Matching both sets of data permits rough estimates
of D, and 8. A transition pore diameter of around
B, = 2 (D, > is found and a surface coverage at steady
state of about 8 = 0.1 emerges.
The dotted-dashed line labelled by straining only
in Fig. 5 reports a calculation assuming the transition
diameter is equal to one drop diameter, and assuming
no interception capture. Equivalently, drops can be
strained only in pores whose throat diameters are less
than their own. This hypothesis is clearly in error and
indicates that interception occurs. Further, intercep-
tion occurs near pore constrictions and then permits
straining in pores whose throat diameters are less than
twice the drop size (i.e. D, - 2 <D, >). We denote this
mode of capture as multi-drop straining.
There is a distinction between multi-drop straining
and the bridging of solid particulates during deep-bed
filtration (Sakthivadivel, 1966; Payatakes and Tien,
1976; Payatakes, 1977; Payatakes and Gradon, 1980).
When a solid suspension flows through a porous
medium, particles are retained not only by the porous
material but also by the previously retained particles.
Since a retained particle protrudes from the pore wall,
it has a greater chance to capture oncoming particles.
Therefore as the process proceeds, particles are cap-
tured largely by the previously retained particles and
form dendrites. These dendrites grow with little inter-
ruption until they connect with others. A dendrite may
build sufficiently to encounter another dendrite on the
opposing side of a pore. Once such a bridge forms, it
may eventually block the pore completely. Due to this
bridging phenomenon, solid particles clog pores of
sizes much larger than the size of the particles
(Sakthivadivel, 1966; Payatakes and Tien, 1976;
Payatakes, 1977; Payatakes and Gradon, 1980).
in which significant repulsion exists among the drops
and grain surfaces, interception capture apparently
occurs only on the porous medium surfaces. Dendrites
do not form and therefore bridging is not possible.
Thus, in emulsion flow, a steady state exists with all
flow in the larger non-straining pores.
For those solid suspensions which can form
dendrites, a steady state is unlikely except at high
flow rates in high-permeability media where bridging
is prevented by hydrodynamic forces. Soo and Radke
(1986) studied the flow of 2.2pm monodisperse poly-
styrene latexes [Dow (No. lAl2)j at ci = 0.005 in the
1.15 pm2 sandpack. The surface charge density of the
stabilized latexes was equivalent to that of the emul-
sion liquid droplets. Few solid particles eluted and no
steady state was achieved. Microscopic examination of
the clogged sandpack revealed the presence of de-
ndrites (Soo, 1983; Soo and Radke, 1986).
In spite of no liquid-droplet bridging, straining of
emulsions is not restricted to pores of throat diameters
smaller. than the droplet diameters. When drops are
intercepted near a throat, they reduce the open pore
diameter. If the resulting throat diameter is smaller
than the diameter of an approaching droplet, the
oncoming drop is then strained out and completely
blocks the pore. By this multi-drop straining mechan-
ism, pores with throat diameters as large as three drop
diameters could possibly plug. However, Fig. 5 reveals
that the actual blocking pore-throat size is close to two
drop diameters.
The amount of interception capture discovered
from Fig. 5 is not large (i.e. 6 equals about 10% at
steady state). This low amount of surface coverage is
reasonable in view of the strong repulsive forces
between the drops and the sand surfaces. A large
portion of the interception capture is probably in dead
 Filtrationmodel for the flow of dilute, stable emulsionsin porous media-11
pore-space caverns or in recirculation eddies.
Interception capture is important and cannot be
discounted, even in situations where straining capture
is significant.
A point worth noting is that for some of the large
drop-size emulsions, in which [In ( DC/p)]/6 is greater
than - 1.5, drop breakthrough is not observed even
after 100 pore volumes of emulsion injection (i.e.
steady state is not achieved). This indicates that the
maximum size of pores in the contiguous void space
through which steady state must be achieved is ap-
proximately equal to the transition throat diameter for
which [ln (D&i)]/& is - 1.5 or D, = ji exp( - l.SS).
Flow-restriction parameter
Equation (6) allows determination
of the flow-
restriction parameter /3 again at steady state:
PO3= (<Bs>++ <BI> <a*,,>)/(%+ <~LIll>).
(13)
where < & > and < & > are the average flow-restriction
parameters in the straining and interception Pore
spaces, respectively. As mentioned earlier in Part I,
<&.> in the straining pore space is around unity.
To estimate the flow-restriction parameter in the
interception region of the porous medium, <& >, we
must calculate the pressure-drop increase across a
constricted tube due to the retained drops. The
pressure-drop increase depends strongly on the pos-
ition of the drop in the constricted tube. Payatakes et
al. (1973) calculate fl, for two types of symmetric
retention patterns. For a smooth monolayer coating
upstream of the pore throat, #I, is about 3, and for a
smooth monolayer coating throughout the pore it is
10. Unfortunately, with the drop sizes dealt with here,
smooth symmetric coatings are not anticipated. An
alternate approach is to consider drops attached to the
surface of the constricted tube. The fluid mechanics for
this case are not available. However, Happel and
Brenner (1965) present results for a spherical particle
in a cylindrical tube. Their results may be transformed,
as outlined in Appendix B, into a value for fir of 13. We
expect & to be larger than this value in a constricted
tube, especially if the drop lodges near the pore throat.
Hence, we arbitrarily take </3, > as between 1S and 20.
Equations (9), (12) and (13) then determine fl, again
with the assumption that fi = pou.
Figure 6 gives the flow-restriction parameter /? as a
function of the dimensionless logarithmic-transition
diameter. The experimental results demonstrate that fl
decreases with increasing drop size, or that small-size
drops are more effective in reducing the permeability
than large-size drops, at the same volume retention.
Similar to the l/a: plot, this figure indicates that
interception capture does exist. If only straining cap-
ture were to occur, /3 = < & > shouId be very close to
unity (Herzig et al., 1970). However, for small drop-size
emulsions, /? is close to 15 showing that interception
capture is dominant. As the drop size of the system
increases, especially in the case that [ln (D&)1/S is
larger than -2, the value of /3 drops to about 3. This
CES41:2--E
279
reveals the increasing importance of straining capture.
Solid lines in Fig. 6 correspond to eq. (13) at several
values of the fractional surface coverage 0 for a fixed
D, = 2<D,> and with <fir> = 18. As in Fig. 5 the
choices of D, and 8 are not unique. Here, however,
increasing D, shifts 8 to lower values (compare the long
dashed line at 0 = 0.1) because more retention in the
straining mode causes less flow restriction (i.e. < & >
c < fl, >). The consequence of this opposing depen-
dence of Q and fi on B is that it is possible to estimate
both D, and 0 from Figs S and 6.
Clearly, the data for the 0.57 pm2 sandpack do not
align with those of the 1.15 pm2 sandpack. It is
possible, by adjusting < /?, >, to effect a better fit of the
OS7 pm data. This is shown by the short dashed line
in Fig. 6 which corresponds to <fir > = 20. However,
altering < & > does not change our conclusion that D,
and 0 are near 2 < D, > and 0.1, respectively.
From the above discussion we conclude that the
filtration model not only explains quantitatively the
experimental results, but also that the phenomeno-
logical parameters A,, , a and /3 can be interpreted
physically. Several of the prediction parameters, in-
cluding 4, <A, >. <Q~,~ > and <fl, >, cannot be as-
signed uniquely, although they cannot be changed by
large amounts from plausibly predicted values.
The results of Figs 4-6 have some very important
ramifications. First, surface capture exists and can
cause straining in pores of throat diameters larger than
the drop diameter. The largest straining pore diameter
is approximately two drop diameters. Second, the
grain surfaces are not completely covered with drops
(i.e. 0 = 0.1). This is probably due to the strong
repulsive drop-sand colloidal interactions. This obser-
vation is sensitive to the surface chemistry of the
system and must not be taken as general. Finally, these
figures explain the increase in retention, or in l/a, with
increasing drop size, and the concomitant decrease in p
with increasing drop size, as found experimentally.
CONCLUSIONS
The theoretical filtration-flow model is quantitat-
ively compared to experimental effluent-drop concen-
tration data and transient permeability data for dilute,
stable oil-in-water emulsions of mean drop sizes
ranging from 1 to 10 pm and with inlet volume
concentrations of 0.5, 0.6, 1.2 and 2.5 0/0 flowing in
unconsolidated quartz sandpacks of about 1 pm*
permeability at constant ionic strength and pH of the
continuous aqueous phase. For emulsion concentra-
tions up to 1.O y0 and for oil-drop viscosities between
1.5 and 23 mPa s, the filtration model successfully
represents the experimental data, permitting direct
evaluation of the phenomenological flow and retention
parameters: rZ,, a and fi.
Theoretical expressions for the filtration parameters
are developed which allow their a priori prediction
given information about the drop size, the pore-size
and grain-size distributions and given some knowledge
of porous medium structure, of interception capture
probabilities and of hydrodynamic resistances of cap-
280 H. so0 er al.

tured particles. The estimation procedures adequately u local oil retention, oil-drop volume/bed volume
reflect the measured experimental parameters in both or local retention of drops in pores of throat
the interception and straining dominated capture diameter D,, m - l
regimes, and they justify why &t increases and why cx r emulsion pore volumes injected, ut/~eL
and fi both decrease with increasing drop size, as
observed experimentally. Additionally, _ the estimation Subscripts
exercise reveals that for repulsive drop-sand grain d droplet ~
interactions little surface capture of drops occurs. Even e emulsion
small interception surface coverages of around 10 %, grain
however, lead to straining in pores of throat diameters : interception
larger than the drop diameters. The largest straining i inlet
pore diameter is found to be around two drop L exit
diameters. m maximum
The filtration theory provides a new tool for under- 0 initial
standing the flow behaviour of dilute, stable emulsions pore
in underground porous media. : straining
SI straining and interception
Acknowledgements-This research was supported by the U.S. t transition
Department of Energy under Grant W-7405-ENG-48 to the W water phase
Lawrence Berkeley Laboratory. H.S. acknowledges financial
co steady state
assistance from the Chevron Oil Field Research Company.
The authors would like to thank Mr. R. F. Hettler of-Dow <> denotes volume average
Chemical Company for supplying the polystyrene latexes.
REFERENCES
Alvarado, D. A. and Marsden, S. S., 1979, Flow of oil-in-water
NOTATION emulsions through tubea and porous media. Sot. Petrol.
twice the particle centre distance to a wall, m Engng J. 19, 369-377.
Devereux, 0. F., 1974a, Emulsion flow in porous solids--I. A
volume concentration of oil drops in emulsion,
flow model. Chem. Engng 1. 7, 121-128.
volume of drops/flowing volume Devereux, 0. F., l974b, Emulsion flow in porous solids-II.
drop diameter, m Experiments with crude oil-in-water emulsion in porous
grain diameter, m sandstone. Chem. Engng J. 7, 129-136.
pore-throat diameter, m Happel, I. and Brenner, H., 1965, Zmv Reynolds Number
Hydrodynamics with Special Application to Particulate
transition pore-throat diameter, m Media. Prentice-Hall, Englewood Cliffs, NJ.
volume fraction of sand grains with diameter Herxig, J. P., Leclerc, D. M. and LeGoff, P., 1970, Flow of
D,, m-i suspensions through porous media-applications to deep
overall permeability, m2 bed filtration. Ind. them. Engng 62, 8-35.
McAuliffe, C. D., 1973, Oil-in-water emulsions and their flow
core length, m
properties in porous media. J. Petrol. Technol. 25.727-733.
unit-bed-element thickness, m Payatakes, A. C., 1977, Model of transient aerosol particle
length of a pore, m deposition in fibrous medii with dendrltic pattern.
pressure, N/m2 A.1.Ch.E. J. 23, 192-202.
time, s Payatakes. A. C. and Gradon, L., 1980, Dendritic deposition
of aerosol particles in fibrous media by inertial impaction
shifted time variable, z - 5 and interception. Chem. Engng Sci. 35, 1083-1096.
velocity, m/s Payatakes. A. C. and Tien, C.. 1976, Particle deposition in
distance, m fibrous media with dendrite-like pattern: a preliminary
reduced axial distance, x/L model. J. Aerosol Sci. 7, 85-100.
Payatakes, A. C., Tien, C. and Tutian, R. M., 1973, A new
model for granular porous medii. A.I.Ch.E. J. 19, 58-66.
Greek letters Pavatakes. A. C.. Tien. C. and Turian. R. M., 1974, Traiectory
flow-diversion parameter &lculation of particle depositions in deep bed fiRration.
how-restriction parameter A.1.Ch.E. J. 20, -905.
flow-restriction parameter of retained drops in Sakthivadivel. R.. 1966. Theorv and mechanism of filtration
of non-colloidal fines through a porous medium. Tech.
pores of throat diameter D, Rep. HEL 155. Hydraulic Engng Lab., University of
variance of Gaussian distribution in In D, California. Berkeley.
bed porosity, void volume/bed volume Soo, H., 1983, Flow of dilute, stable emulsions in porous
porosity contribution of pores of throat dia- media. Ph.D. Thesis, University of California, Berkeley.
Soo, H. and Radke, C. J., 1984, The flow mechanism of dilute,
meter D,, m-l
stable emulsions in porous media. Jmf. Engng Cheer.
drop capture efficiency in pores of diameter D, Fundam. 23, 342-347.
fraction of monolayer coverage Soo, H. and Radke, C. J., 1986, Flow of dilute, stable liquid
filter coefficient, m-i and solid dispersions in underground porous media.
reduced dimensionless filter coefficient, rZL A.I.Ch.E. J. (in press).
Thomasian, A. J., 1967, The Structure of Probrrbifity Theory
viscosity, mPa s with Applications. McGraw-Hill, New York.
ln F is the mean of the Gaussian distribution Tien, C. and Payatakes, A. C.. 1979, Advances in deep bed
in In D,, m filtration. A.I.Ch.E. J. 25, 737-759.
 Filtration model for the flow of dilute, stable emulsions in porous media-II 281

APPENDIX A. PARAMETER DETERMINATION At early injection times (T > 1) both bi and cL are very much
This appendix indicates how the filtration parameters less than ss, so that eq. (19) of Part I becomes:
AsI. a and fl are determined from the emulsion flow data. 1
KO
-gp++ AG In (ai/ by)
Since the reduced filter coefficient A,, and the flow-diversion L48)
parameter .x reflect the processe s of the drop retention in the K(r) (l-_/x) (l-a/B) (I+xci) .
sandpack, they should be evaluated from emulsion Substituting cJcL for ui/uL from eq. (2), and using
breakthrough data. The flow-restriction parameter fi. which ln(cL/Ci) nAsr(l -acir) from eq. (A7), we obtain
characterizes how effective the retained drops are in reducing
permeability, is found from pressure-drop data.
First, we relate the inlet and outlet concentration datain the -zKO B
1+ -Ci(T+l)r fA9)
form of the ratio cL/ci. Since eq. (2) shows that cL/ci = uL/ui, K(r) 1-8/e
the next step is to evaluate uL and cri.From eq. (I), with T(L) where we have also neglected higher-order terms in xei, which
=s-landT(O)=r,wehave is assumed to be small. This expression can be fitted to data in
a plot of K,/K vs. ci7 to obtain p/(1 - /?/a) from the slope at
1 - exp [aAs,ci (r - l)]
-=
CL=
(Al) short times. This, combined with a determined by other
&Cl 1 - exp As, - exp [ahsrc; (T - l)] methods, yields 8. The problem here is that a cannot be
and determined from eq. (A4) as before, if breakthrough (cL/ci
uia
- exp [aAstcir] - 1 (A2)
= 0.5) does not occur. In such a case, one hnds a by exercising
,- exp [aAsrcir] . judgement in reconciling estimates based on a projected K,
jthus using eq. (A6) and fits of the short-time data in terms of
Division of these two expressions yields:

(1 -exp [aAsrci(r - l)])exp (aAsIcir)

~-
UL CL - (A3)
ui ci (1 -exp As,-exp [aAsrci(z - I)]) [l -exp (aAsicir)] .

Since drop/sixes and pore sixes in this study are about the
same order, a large value of the filter coefficient is anticipated.
Under this circumstance exp Asr * 1 and capture occurs in a
sharp front.
Next, we focus on the breakthrough region and, in
particular, consider the point where cL/ci = 0.5. As will be
justified below, this condition requires that
aci(r-I)= 1,
independent of the value of As,. In such a case, terms in eq.
(A3) that contain products such as Ax, aci (r - 1) become of
order AsI and thus all exponentials in that equation exceed
unity greatly. (Clearly, long times are implied here, so that
r - 1 and r have similarly large magnitudes.) Under these
conditions, eq. (A3) simplifies to:
K (r)]. Fortunately, the latter is not sensitive to the value of
the very large As), so computed values of a and fl are not
influenced significantly by it.
APPENDIX B. DROPLET FLOW RESTRICTION IN A
CYLINDRICAL PORE
(A4) This appendix calculates the average flow-restriction par-
ameter in the interception pores, <& >, from a mode1 of a
spherical drop resting on the inside surface of a cylindrical
pore. Happel and Brenner (1965) give the increased pressure
drop AP* due to the presence of a single, stationary solid
sphere in a cylindrical tube (not necessarily at the wall) under
creeping Row [see also Payatakes (1977)]:

exp CaAstci (r - 240, u

CL
-=
1))
(A5)
=i exp A,, + exp [aAsrci (r - l)]
Note that this function assumes the value 0.5 precisely when
eq. (A4) holds, thus providing the justification promised
above. The point cL/ci = 0.5 in the efIIuent-concentration
history is used to specify the flow-diversion parameter a,
according to eq. (A4). Once a is known, Ast may be obtained
by a best fit of the entire emulsion effluent volume concen-
tration history via eq. (A5).
The flow-restriction parameter p is found from the steady-
state permeability:
K,fK, = 1 -$/a. (A6)
With a known, fi follows directly from the measured value of
K,/Ko. This parameter estimation procedure does not
involve the entire unsteady permeability behaviour. Only the
steady-state pressure in combination with the elIIuent emul-
sion volume concentration is required.
An exceptional case arises when the drop sixes are so large
compared to the pore sixes that emulsion breakthrough does
not occur within an experimentally conveniet time frame. In
this situation, the value of 01is small while the value of A,,
remains large. Furthermore, in this case we consider rather
short times in the sense of r z 1. Thus, we have the dual
conditions: exp Ast 9 1 and exp [a Asrcis] g 1. Hence, eq.
(A3) can be written as:
CL exp (aAs ci + )/exp As,. (A7)
ci -
AP=- l-(Dp--;)) (I+;&, (Bl)
D;
where b is the twice the distance from thecentre ofthe particle
to the tube wall. Equation (Bl) applies to a liquid drop as long
as the droplet surface is laden with enough surfactant to
support the no-slip condition. For a drop attached to the
wall, b = Dd. Now, when Darcys law along with the
Hagen-Poiseuille result for the pressure drop in an open tube
of length L is used to predict AP,, and thus define K,, then
combination with eq. (Bl) (i.e. AP = AP, + AP*) yields an
expression for the permeability reduction:
K
-43(3)(2-3. (B2)
KO
We recognize that U/E,, is proportional to the ratio of the drop
volume to the tube volume. With this observation, com-
parison of eq. (14) of Part I and eq. (B2) gives the desired
result:
&=:(2-$)ls 14(1-s)l. (B3)
For the ease of D, 4 D,, j?, = 14. If we take the mean drop-
sixe to pore-size ratio to be 0.1, then & = 13. Equation (B3)
indicates that smaller drops are more effective in reducing
permeability on a unit volume retention basis, in that &
decreases with increasing drop size. This is consistent with the
experimental findings of Table 1 and Fig. 6.