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1967-Frankel, Acrivos-On The Viscosity of A Concentrated Suspension of Solid Spheres
1967-Frankel, Acrivos-On The Viscosity of A Concentrated Suspension of Solid Spheres
1967-Frankel, Acrivos-On The Viscosity of A Concentrated Suspension of Solid Spheres
N. A. FRANKEI.and ANDREASACRIVOS
Department of Chemical Engineering, Stanford University, Stanford, California
Abstract-An asymptotic technique is used to derive the functional dependence of effective viscosity
on concentration for a suspension of uniform solid spheres, in the limit as concentration approaches
its maximum value. This result, containing no empirical constants, is intended to complement the
classical Einstein formula which is valid only at infinite dilution. Good agreement is found between
the asymptotic solution and available data, provided that the maximum concentration is determined
from the data themselves.
847
N. A. FRANKEL
and ANDREAS
ACRIVOS
1
“= 1(2n - 1)(2n + 3)
or,
4 cosh*(n + +)a + (2n + l)*sinh*a _ 1
2 sinh(2n + l)a - (2n + 1)sinh 2a (3)
with
%i I:
as -+O
E-2npW*a[ -$-2+(2+$45+)j
FIG. 1 (12)
Equations (l), (3) and (5) then specify quite which in turn reduces to
generally the rate of viscous dissipation of energy --
in either half-space for all a and W, consistent with E-3rcpW’a a
the equations of creeping motion. However, of 11
particular relevance to our problem is the asymp- when h/a-+0. This expression is of course identical
totic solution in the limit h/a+O, implying a+O, to Eq. (9), a fact which confirms our contention
848
On the viscosity of a concentrated suspension of solid spheres
that only the gaps need be considered in the vanish or are negligibly small for viscometric flows.
asymptotic limit h/a-+0. This velocity field is identical for all Newtonian
A lubrication type analysis can also be applied fluids and must therefore characterize the motion
to the case of sliding relative motion of two spheres. of the suspension in a macroscopic sense. We shall
Referring once more to Fig. 1, with the sphere henceforth refer to it as the continuum field.
velocities now directed parallel to the line y= z=O, Furthermore, in accordance with our earlier
we find for the local rate of dissipation in the gap assumption that the spheres of the suspension
w= (13)
behave as fluid particles, we can express the
relative velocity between the i-th sphere and a
(D-lh+2a(l-Jl-r2/a=)]= neighbor by means of
in which, terms of the order of the curvature of the a$=di. ri (17)
bounding surfaces have been neglected. The rate
of viscous dissipation of energy is thus where d’ is the continuum rate of strain tensor
)I
evaluated at the center of the i-th sphere and
E+dJ2 -2a+(2a+h)lo 1,; (14) ri is the position vector drawn to the center
[ 8( of the neighbor. The squared velocity W2,
which, as h/a-+0, is clearly of smaller order than which appears in the asymptotic expression (9),
the term given earlier by Eq. (9). Hence, we shall can be related to the tensor field d by making
neglect the contribution from this type of motion. use of Eq. (17) and averaging over possible orienta-
tions of neighboring spheres. This averaging is
3. LIMITINGEXPRESSION FOR THE EFFECTIVE particularly straightforward if we assume either
VISCOSITY that all orientations are equally likely, or that six
Following BRENNER [6], we now define the of the neighbors are aligned along the principal
effective viscosity of a suspension as directions of strain, obtaining in both cases
P*_
-- Js,(a*l-l * es ; v=v(O) on So (15)
< W= > =A(2a + h)=(d’ : d’) (18)
p j&&l * l-I(“) * v’O’)dS where, respectively, A = l/30 or A = l/l 2. Equa-
in which the right-hand side denotes the ratio of tions (9), (16) and (18), when combined, yield then
the rates of work being performed by the stresses for the effective viscosity
at the boundaries of an apparatus containing,
respectively, the suspension in question or an 3zfia(2a+h)= ; -$di : d’
equivalent volume of pure liquid. This definition LAN 0
(19)
P 2&d : d&’
is consistent with the usual experimental methods
for determining viscosity, such as Couette vis- where N is the number of neighbors of each sphere
cometry. Furthermore, because of the steady contributing to the asymptotic dissipation rate
nature of the flow in these instruments, the drags and the summation is over all spheres within the
and couples on small particles tend to vanish, so apparatus. For the case of small particle-apparatus
that Eq. (15) becomes equivalent to volume ratios, however,
where the subscript T denotes the total rate of to a high degree of approximation, so that Eq. (19)
viscous dissipation of energy within the confines of reduces to the simple form
the apparatus.
CL*-C!
The boundary condition v= v(O) on So is suffi-
cient to specify the velocity field at all points
within So independent of the viscosity, since the
P 0h,
asLO
a
(20)
849
N. A. FRANKEL and ANDREAS ACRIVOS
In order to compare Eq. (20) with existing models We shall further assume that the shear flow on a
and with available data and correlations, it is con- macroscopic scale is given by
venient to express the quantity u/h in terms of the
concentration of the suspension. We shall assume u = it/2X
that this functional dependence is the same as that v = lc/2y (23)
for cubic arrangements of spheres, yielding
w= --KZ
which is the principal result of this work. Referring to Fig. 2, we see now that the neighboring
spheres shown there have the instantaneous velocity
4. DETERMINATIONOF THE CONSTANT C’ values U= (2a+ h)rc/2 and that two additional
The precise determination of the value of C’ is nearest neighbor spheres exist with velocity vectors
an elusive problem and it is likely that a statistical directed inwards towards the central sphere and of
treatment would be necessary at this point. For- magnitude (2a+h)rc. Other spheres of the suspen-
tunately, however, a cage model similar to that of sion are situated in some random fashion. Adding
SIMHA [7] is found to yield a value for C’ giving the contributions from the six neighbor spheres
good agreement with available viscosity data. The which are given by Eq. (9), we find for the rate of
cage is taken to consist of a particle surrounded energy dissipation in the cell,
instantaneously by a cubic configuration of neigh-
boring particles (shown in Fig. 2) which is then E cell +72a + h)2a ;
replaced by a spherical cell representing the 0
“region of influence” of the particle in question. while, for an equivalent spherical cell of homo-
In other words, the velocity field on the boundary geneous liquid, undergoing the rate of strain
of the spherical cell is supposed to be equal to that indicated by Eq. (24), the rate of dissipation is
on an equivalent surface in a pure liquid under-
going the same macroscopic shearing flow. E homogeneous = 3pn’b + h/2)‘] (26)
c_
P 0
9a
G
so that, from Eqs. (21) and (22)
as h/a+0 (28)
C’ = 918 (29)
It should be stressed at this point, though, that
850
On the viscosity of a concentrated suspension of solid spheres
5. COMPARISON
WITH EXPERIMENT
AND
OTHER THEORIES 6o - Jtulgerr (averagecurve)
6. _ &= 0.535
Viscosity data for suspensions of solid spheres &Thomas (reduced data 1
are quite numerous, but, unfortunately, the agree-
ment among the various investigations has been
rather poor in the high concentration regime. A
number of reasons have been proposed for these
conflicting results: wall effects in capillary visco-
meters, slip at particle surfaces, insufficient dis-
persion, adsorption, turbulence, sedimentation,
non-Newtonian behavior, etc. THOMAS [3] has Einstein- Simha
recently considered some of these problems, and
by appropriate extrapolation techniques, was able
to minimize non-Newtonian, inertial and non-
homogeneous effects and to fit the resulting
adjusted data to a smooth viscosity curve with
little scatter. Also, an attempt to sort out the
more reliable measurements was made by RUTGERS
[2] whose average curve, although quite arbitrary,
is in good agreement with the data of the (appar-
ently) most careful investigators.
FIG. 3
The data of Thomas and of Rutgers have been
plotted in Fig. 3 together with the asymptotic
expression, Eq. (22). In order to determine the
maximum concentration in each of the two cases,
we adopted a suggestion of Thomas which was to
IOO-
plot [(p*/p)- 11-l vs. cp and extrapolate to zero
60-
ordinate. The asymptotic expression is seen to 0 Rutgers (average curve)
60 - A Thomas (reduced data
agree quite well with the measurements for con-
centrations greater than eight-tenths of the maxi- 40-
mum, which corresponds to h/u= 0.16.
Also shown in Fig. 3 is the EINSTEIN[I] result,
20-
valid for infinite dilution and the quadratic correc-
tion as calculated by GUTH and SIMHA [8] and P
Y_
851
N. A. FRANKEL
and ANDREAS
ACRIVOS
have been proposed for highly concentrated sus- Acknowledgment-This work was supported in part by the
National Science Foundation.
pensions. We summarize here, several of the best
known models, one of which is totally empirical:
SIMHA [7]. The parameter f is empirical, 1 <f c2 NOTATION
radius
dimensionless number
dimensionless number
rate of deformation tensor
MOONEY [I 01. The parameter K is empirical, 1.35 I
rate of viscous dissipation
KS I.91 empirical constant
frictional force
minimum gap width
unit outer normal
number of nearest neighbors
EILERS[I 11. The entire expression is empirical radius in cylindrical coordinates
position vector from origin of i-th particle
(32) to that of a neighbor
boundary of viscometric apparatus
increment of surface area
Simha’s analysis is based on the idea that the X, y and z velocity components, respectively
neighbors of each sphere in the suspension can be velocity, defined in Fig. 1
replaced by a rigid spherical wall, while the Mooney velocity vector
relation is similar to one originally proposed by velocity on S,
volume
ARRHENIUS [13] with the addition of a crowding
velocity, defined by Eq. (2)
factor, 1 - Kcp. Cartesian coordinates
The present result is believed to be a funda- gap width, a function of distance from the
mental improvement over existing models since it line of centers
has been developed without recourse to empiricisms defined by Eq. (4)
Stokes correction, defined by Eq. (1)
or artificial boundaries. This result also indicates
increment of velocity
that the rapid rise of viscosity which is observed at shear rate
high concentrations can be accounted for solely by viscosity of pure liquid
the hydrodynamic interactions of neighboring effective viscosity
spheres. We presume, therefore, that collisions, stress tensor
concentration (volumetric)
aggregation and inertial effects are of minor
the local rate of viscous dissipation per unit
importance in the usual experimental arrange- volume, defined by (9=2pd:d, for an
ments. incompressible fluid
REFERENCES
111 EINSTEIN
A., Ann. Phys. 1906 19 289; Ann. Phys. 1911 34 591.
PI RUTGERS IR. R., Rheof. Actu 1962 2 202, 305.
[31 THOMAS D. G., J. Colloid Sei. 1965 20 267.
[41 BRENNER H., Chem. Engng Sci. 1962 16 242.
[51 LANDAU L. D. and LIFSHITZ E. M., Fluid Mechanics Vol. 6, p. 70, Pergamon Press 1959.
161 BRENNER H., Phys. Fluids 1958 1 338.
171 SIMHAR., J. Appl. Phys. 1952 23 9, 1020.
PI GUTH E. and SIMHAR., Kolloid Zh. 1936 74 266.
191 SAITON., J. Phys. Sot. Japan, 1950 5 4.
[toI MOONEYM., J. Colloid Sci. 1951 6 162.
f111 EILERSH., Kolloid Z. 1943 102 154.
U21 JOLLEYL. B. W., Summation of Series, pp. 383, 764, 224, 766, Dover 1961.
1131 ARRHLENIUS S., Z. Phys. Chem. 1887 1 285.
852
On the viscosity of a concentrated suspension of solid spheres
SE f
n(n + 1)
n= 1(4n2- 1)(2n - 1)(2n + 3)2
1
-3/g l/64
=J (2n - 1)2(2n + 3)2 - (2n - 1)(2n + 3)
?(2n+l)-‘(2n+3)-‘=1/6
1
Therefore,
Zusannnenfassnng-Zum Ableiten der funktionellen Abhlngigkeit der effektiven Viskositat von der
Konzentration in einer Suspension gleichformiger, fester Kugeln-innerhalb des Bereiches, in dem sich
die Konzentration ihrem Hiichstwert nahert-wird eine asymptotische Technik angewandt. Das
Ergebnis, das keine empirischen Konstanten enthllt, sol1 die klassische Einsteinformel erganzen, die
nur in unendlicher Verdtinnung gilt. Zwischen der asymptotischen Losung und den zur Verftigung
stehenden Daten wurde gute Ubereinstimmung gefunden, vorausgesetzt, dass die Hochstkonzentration
aus diesen Daten selbst bestimmt wird.
853