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Fluid Dynamics Research 40 (2008) 565 – 575

Increase of effective viscosity in bubbly liquids from transient

bubble deformation
Yuichi Muraia, b,∗ , Hiroshi Oiwaa, b
a Graduate School of Engineering, Hokkaido University, Sapporo, Japan
b Fuji Heavy Industry, Co. Ltd, Mitaka, Japan

Received 27 November 2007; received in revised form 21 December 2007; accepted 21 December 2007
Available online 18 April 2008
Communicated by S. Fujikawa

Abstract
The effective viscosity of bubbly liquids is measured using the Stokes drag of a falling sphere, i.e. falling sphere
viscometry. This method can evaluate the influence of a bubble’s transient deformation. Viscosity relative to a
single-phase fluid is directly obtained by the terminal falling velocities of the sphere. When bubbles are distributed
around the sphere up to a void fraction of , the following results are obtained. The relative viscosity for spherical
bubble dispersion agrees with the Stokes–Einstein formula; 1 + . For large capillary numbers, relative viscosity
converges to approximately 1 − (5/3) because bubble deformation is fully yielded. Between these two states,
relative viscosity has a value higher than in simple shear flow. The critical capillary number is found to be 3.5, being
five times as that of simple shear flow. The viscosity-increasing mechanism for trans-critical capillary numbers is
deduced from the fact that bubbles have transient deformation along the streamline.
© 2008 The Japan Society of Fluid Mechanics and Elsevier B.V. All rights reserved.
Keywords: Viscosity; Rheology; Shear stress; Deformation; Falling sphere viscometry

1. Introduction

Effective viscosity of suspension, such as that for bubbles, drops, and solid particles is described as
a function of the volume fraction of the dispersion. Einstein (1906) derived theoretically the effective
∗ Corresponding author at: Graduate School of Engineering, Hokkaido University, Sapporo, Japan. Tel.: +81 11 706 6372; fax:
+81 11 706 7889.
E-mail address: murai@eng.hokudai.ac.jp (Y. Murai).

0169-5983/$32.00 © 2008 The Japan Society of Fluid Mechanics and Elsevier B.V. All rights reserved.
doi:10.1016/j.fluiddyn.2007.12.009
566 Y. Murai, H. Oiwa / Fluid Dynamics Research 40 (2008) 565 – 575

viscosity of a dilute particle suspension, , to be

 = /0 = 1 + 25 , (1)

where 0 and  are the viscosity of the continuous phase and the volume fraction of the dispersion. Taylor
(1932, 1934) proposed the following formula that is applicable not only to solid particles but also to
bubbles and drops as the dispersion phase:
0 + (5/2)
 = /0 = 1 + , (2)
0 + 

where  stands for the viscosity of the dispersion phase. Batchelor explained this important law in a
book and a paper (Batchelor, 1967, 1970). Nowadays this formula is widely used in fluids and chemical
engineering (e.g. Tsuchiya et al., 1997). For gas bubbles, dispersion viscosity is negligible in comparison
to that of liquid, and hence Eq. (2) is approximated to be

 = /0 = 1 + . (3)

Most of numerical simulation models to date employ Eq. (3) as the first-order approximation of the
bubble influence on effective viscosity (e.g. Kitagawa et al., 2001). This is, however, only valid for
spherical bubbles, i.e. for low capillary numbers. When bubbles exist densely as in foam, the high surface
tension caused by the complicated liquid film governs the macroscopic viscosity and induces visco-elastic
properties (Tisne et al., 2003; Xu and Rossen, 2003; Kuvalchuk et al., 2005; Hoehler and Cohen-Addad,
2005; Denkov et al., 2006). When bubbles are deformed, the surrounding shear stress changes as a function
of capillary number:
rG GL
Ca = , (4)

where , rG and G are the surface tension, bubble radius, and shear rate. The magnitude of bubble
deformation in simple shear flow was investigated by Rust and Manga (2002a, b). For high viscosity
fluids, Ca number easily increases even for low shear rate. Ca number dependence on shear stress is often
analyzed for research in geophysics, e.g. for estimating the dynamic properties of magma and volcanoes
(Pal, 2003). For pressure-driven bubbly flow, bubbles produce pseudo-turbulence that modifies shear
stress drastically. In such cases the effective viscosity cannot be defined because it should be separated
from the eddy viscosity.
This study aims to investigate effective viscosity in homogeneous bubbly liquids subjected to strong
shear. For this condition, Frankel and Acrivos (1970) proposed a theoretical estimation of relative viscosity
as
1 − (12/5)Ca2
=1+ . (5)
1 + ((6/5)Ca)2
This formula tells us that relative viscosity falls below unity for Ca > 0.65; one explanation for this is
that viscosity is reduced for bubble stretching (Hinchi and Acrivos, 1980). This criterion at which  gets
less than unity is called the critical Ca number. Under this condition, the bubbles in a boundary layer
produce a shear-thinning effect whereas spherical bubbles thicken the boundary layer (Legner, 1984).
 Y. Murai, H. Oiwa / Fluid Dynamics Research 40 (2008) 565 – 575 567

Schowalter et al. (1968) obtained the following formula valid for the higher void fraction bubbly
liquid:
1 + ( 65 Ca)2 (1 + 3 )(1 + 4)
20
= (1 +  + 25 2 ). (6)
1 + ( 5 Ca) (1 + 3 )
6 2 20 2

Taking the Maclaurin expansion in terms of  to obtain the leading order, gives us the same result as Eq.
(5) for the critical capillary number. They concluded that the relative viscosity is well approximated by
Eqs. (5) and (6). Manga and Lowwenberg (2001) analyzed a possible range of the viscosity change in
steady shear flow using this formula, and concluded that it achieves up to 50% of the original viscosity.
These theoretical formulae were validated experimentally by Rust and Manga (2002a, b) using circular
Couette flow experiments. Llewellin and Manga (2005) demonstrated the validity of these formulae by
analyzing the modification of a steady laminar pipe flow containing bubbles.
The above-mentioned studies dealt only with a steady deformation of bubbles in simple shear flow, and
thus do not universally express the general behavior of effective viscosity. The viscosity of bubbly liquids
that involve bubble’s transient deformation has not been investigated yet so far. Here the word “transient
deformation” is used for the bubbles that have time-varying deformation ratio. This unsteadiness takes
place due to several factors: (1) time lag between the surface tension-originated elastic stress and the
shear stress around the bubble, (2) inertia of liquid around the bubble, and (3) other non-equilibrium
phenomena of the interface in molecular scale. We deal with the first factor in this paper, i.e. the influence
of delayed deformation for rapid change in the shear stress.
There are a number of viscometers, with various principles, proposed and used to date. Examples
include: use of Poiseuille flow in tube, Couette flow in rotating disk, and Stokes flow around a sphere.
The last method is called “falling sphere viscometry” and measures the viscosity of the target fluid based on
Stokes drag theory (Stokes, 1851). Falling sphere viscometry is used in various industrial fields, including:
petroleum transport, food processing, liquid metal flow and other chemical solutions. In the sedimentation
prices for separating dispersions from mixtures, viscosity estimated by the falling sphere method best
predicts the necessary processing time. Nyugen and Evants (2003) investigated flow alternation around
a sphere moving in a bubble suspension. Rees et al. (2005) measured the terminal velocity of a sphere in
a bubbly fluid containing a particulate suspension to investigate drag modification.
In this paper we discuss the effective viscosity of bubbly liquids that do not exhibit steady deformation,
say, non-Newtonian properties. We find that the effective viscosity increases considerably with the La-
grangian deformation rate of bubbles when the surface tension and viscous shear stress are competitive.
This increase in viscosity can produce a thickened boundary layer in a tube, and delayed sedimentation
in bubbly liquids. This effect is also associated with turbulent flow control since local turbulent eddies
containing bubbles can be modified or suppressed by local increases in viscosity.

2. Falling sphere viscometry

One of the advantages in falling sphere viscometry is that the target fluid can be kept quiescent, and
hence the fluid is entirely free from external stress. Various types of rotating viscometer generate radial
pressure gradients from centrifugal acceleration and make bubble distribution non-uniform. The falling
sphere method does not need to drive the fluid, so the quality of bubbly mixture (i.e. bubble diameter and
the spatial distribution) is better controlled than in other methods.
568 Y. Murai, H. Oiwa / Fluid Dynamics Research 40 (2008) 565 – 575

Fig. 1. Schematic diagram of experimental apparatus.

2.1. Experimental setup

Fig. 1 shows a schematic diagram of the experimental apparatus. The container is 100 × 100 × 700 mm
and made of transparent acrylic resin. The liquid used in this experiment is Silicone oil with kinematic
viscosity of 5 × 10−3 m2 /s at 25 ◦ C. Bubbles are generated through a porous body from the bottom of the
container and mixed uniformly using mechanical fans. The void fraction is measured from the upheaval of
the top surface, i.e. hold up. The bubble diameter is measured by image processing of local photographs.
The test spheres are steel balls of 7800 kg/m3 with radii from 3 to 8 mm. The test sphere is released from
a position just below the top surface using an electromagnet so that the initial velocity is controlled to be
zero both in translational and rotational motions. Table 1 shows the detailed experimental conditions.
Fig. 2 shows a sample of consecutive images of falling spheres with 16 mm in diameter. The large
solid circle is the shadow of the sphere and the ambient dots are the shadows of the bubbles. As shown in
the pictures, the terminal velocity of the sphere depends on the void fraction, . The terminal velocity is
measured by image processing based on cross correlation analysis. The Reynolds number of the falling
sphere is less than unity. The bubbles’ rising velocities are negligibly small and their Reynolds numbers
are less than 1/500. The ratio of bubble to sphere diameter ranges from 0.1 to 0.3, and the bubbles are
much smaller than the length scale of the liquid flow in Stokes flow regime.

2.2. Measurement of effective viscosity

For a falling sphere at terminal velocity, the following force balance is satisfied:

3 rS ( − 
¯ )g = CD rS2 21 ¯ U2 .
4 3
(7)
Here the average density of fluid around the sphere is expressed as
¯ = L (1 − ) + G . (8)
 Y. Murai, H. Oiwa / Fluid Dynamics Research 40 (2008) 565 – 575 569

Table 1
Experimental conditions

Container, liquid and sphere conditions

Container width W 100 mm
Container height H 700 mm
Liquid density L 973 kg/m3
Kinematic viscosity L 5 × 10−3 m2 /s
Sphere radius rS 3–8 mm
Sphere density S 7810 kg/m3
Sphere Re number Re 0.001–0.43
Bubble conditions
Surface tension  21.3 mN/m
Bubble radius rG 1.0 ± 0.15 mm
Void fraction  0–0.030
Gas density G 1.21 kg/m3

Hence the drag coefficient is measured by

 
8 S gr S
CD = −1 . (9)
3 ¯ U2
The Stokes drag law is written as
A A
CD = = , (10)
Re 2¯rS U
where  is the effective viscosity and A is the Stokes constant which is known to be 24 for a solid sphere.
Eqs. (9) and (10) give the effective viscosity to be
16(S − ¯ )gr 2S
= . (11)
3AU 
In bubble-free liquid, Eqs. (8) and (11) lead to the viscosity 0 as
16(S − L )gr 2S
0 = , (12)
3A0 U0
where U0 is the terminal settling velocity of a sphere in single-phase fluid.
A and A0 in Eqs. (10) and (12) are treated as the same because of the definition of effective viscosity,
i.e. the change in drag coefficient for bubbles is interpreted as change in viscosity. This means that the
value A depends only on the boundary condition and not on property of fluid. From Eqs. (11) and (12),
the relative viscosity is obtained as
 −1  −1  
 U S − ¯ U 1− G S G
= = = 1+  , S= , G= . (13)
0 U0 S − L U0 S − 1  L L
The coefficient of the void fraction  in the above equation is constant, and is 0.147 in this experiment.
The relative viscosity is obtained from Eq. (13) after the terminal velocity of the sphere and the average
void fraction are measured.
570 Y. Murai, H. Oiwa / Fluid Dynamics Research 40 (2008) 565 – 575

Fig. 2. Falling spheres in bubbly liquid.

Fig. 3. Drag coefficient and Reynolds number of a falling sphere.

2.3. Measurement uncertainties

In this section, the quality of the measurement is declared briefly. (a) Accuracy of settling velocity
measurement: The position at which the steel sphere reaches its terminal velocity can be estimated by a
motion equation that constitutes of inertia, added mass, gravity, drag, buoyancy, and history forces. The
estimated position at which the sphere reaches 99.99% of terminal velocity is obtained as 35 mm from
the release point of the sphere. Thus, we set the measurement position at 200 mm below the release point.
The velocity is measured by image cross correlation analysis. The sphere is more than 200 pixels in size
in the digital image so the measured center of gravity is negligibly affected by the image resolution. It
is noted that the velocity cannot be measured when the void fraction gets higher than 3% because of the
optical limitations of capturing the motion of the sphere in the backlight image.
(b) Wall-confining effect: While the Stokes drag law is used to obtain effective viscosity, the exact
Stokes flow requires infinite space around the sphere. Fig. 3 shows the drag coefficient of bubble-free
liquid, measured in the present container. The plots from A to E are the measured values for different
spheres which are shown above the graph, and the dotted line is the interpolated function in the range
 Y. Murai, H. Oiwa / Fluid Dynamics Research 40 (2008) 565 – 575 571

tested. The data are slightly higher than the theoretical values for Stokes and Oseen drag coefficients
owing to wall confinement. This discrepancy gradually increases as the Re number gets larger. This trend
is explained by the size effect, i.e. a large sphere with a higher Re number is more strongly affected
by the wall. Nevertheless, the measurement of relative viscosity is unaffected by wall-confinement even
though the absolute drag increases due to the presence of wall. This is because the wall-confining effect
is accounted for by change of Stokes constant A, rather than change of fluid properties. This is confirmed
by the form of Eq. (13), and is an important advantage of falling sphere viscometry.

3. Experimental results and discussion

Measurement results for relative viscosity are shown and discussed in this section. The relative drag
coefficient is simply derived from Eqs. (8) and (13) as
CD ( S − 1){1 − (1 − G )}
= 2 . (14)
CD0 S − 1 + (1 − G )

This paper only presents the results for relative viscosity. The relative drag coefficient is not shown
because it is self-evident given the above equation from the relative viscosity, .

3.1. Relative viscosity as a function of void fraction

Fig. 4 shows how relative viscosity changes with void fraction and sphere diameter. Each experimental
plot corresponds to a single drop test, and cubic spline curves are superimposed on the diagram for easier
identification of trends in the change. These spline curves are obtained to connect the arithmetic averages
taken for each void fraction. A gray solid line is the theoretical relative viscosity for spherical bubbles
given by Eq. (3). The following remarks are found with the results: (1) relative viscosity increases with
void fraction for spheres smaller than 8 mm. The slope of the increment roughly agrees with Eq. (3).

Fig. 4. Relative viscosity as a function of void fraction.

572 Y. Murai, H. Oiwa / Fluid Dynamics Research 40 (2008) 565 – 575

Fig. 5. Viscosity factor f as a function of Ca number.

(2) The viscosity changes non-monotonically with void fraction for spheres larger than 10 mm, or rather
decreases as void fraction increases. The large deviation in the data is an inevitable feature of dispersed
multiphase fluids and is not due to measurement error. That is, the number of bubbles affecting the falling
sphere is limited. Therefore only the mean viscosity is going to be discussed hereafter.

3.2. Relative viscosity as a function of capillary number

Capillary number, Ca, is a dimensionless shear stress relative to the surface tension of bubbles. It is
defined by the following formula in this study:
rG GL rG L U U
Ca = = , G= . (15)
  rS rS
The shear rate, G, of the fluid around the falling sphere is approximated to the sphere velocity divided
by sphere radius. The relative viscosity is approximated to be a linear function of void fraction as

 = 1 + f . (16)

This approximation is valid for low void fraction and thus the factor f is obtained from the experimental
value as

f = ( − 1)/. (17)

When f is negative, viscosity decreases with the presence of bubbles. When f is zero, the resultant stress
field around the sphere is insensitive to the drag. The capillary number that causes this condition is defined
as the critical Ca number.
Fig. 5 shows the measurement results of f , as a function of Ca number. Individual experimental plots
are the averaged over more than 50 iteration tests, and the error bar indicates the standard deviation. The
thick solid curve is the theoretical viscosity factor for Couette flow, referred to Eq. (5) in Frankel and
Acrivos (1970). The dotted curve is a Gaussian fitted value of the present measurement result, which
 Y. Murai, H. Oiwa / Fluid Dynamics Research 40 (2008) 565 – 575 573

is obtained as
        
42 5 18 2 5 18 2
f =1+ exp − Ca − − exp − . (18)
11 19 13 19 13
This formula satisfies f = 1 at Ca = 0, and f = −5/3 at a Ca of infinity. Note that this is an experimen-
tal fitting formula and not derived from any theoretical base. We propose this formula for the viscosity
factor f in Stokes flow. The most important result found from the data is that the critical capillary
number is obtained as Cac = 3.3 and is five times that for Couette flow (Cac = 0.65). This means that
the bubble-yielding mechanism in Stokes flow around a sphere is different from that in simple shear
flow. The second point is that f becomes larger than unity around Ca = 2. This is not explained by
the magnitude of the Ca number alone and we have to reconsider the mechanism from a new point of
view.

3.3. Bubble deformation around a falling sphere

The Stokes flow around a sphere is theoretically given by the following equations:
 
3 rS 1 rS3 3 rS 1 rS3
ur = U cos 1 − + , u = U sin 1 − − . (19)
2 r 2 r3 4 r 4 r3
Here, r and are the radius from the center of sphere and the angle from the front stagnation point,
respectively. The area-average shear rate on the surface of the sphere is

1 ju U
Gw = 2 (2rs2 sin ) d = . (20)
4rs2 0 jr r=rs 3 rs
The gap between Eqs. (15) and (20) is smaller than 5%. This implies that the drastic difference in
critical capillary number found in this experiment may not be due to the selection of the referential shear
rate.
Fig. 6 shows the bubble deformation pattern around a falling sphere at Ca = 3.3; the present critical
capillary number. Here shown are (a) the distribution of shear strain rate normalized by U/rs , (b) an
experimental photograph of single bubble deformation, and (c) numerical results of bubble deformation
on the Stokes flow field at the same Ca number. The numerical results are calculated by marker advection
method, i.e. calculating the Lagrangian interface displacement on liquid advection, on which the elastic
force due to surface tension is delivered. The bubble in the upstream region (i.e. the bottom of sphere)
has a nearly spherical shape, and gradually deforms as it passes near the side surface of the sphere. The
bubble in the downstream region is considerably elongated. The longitudinal axis of the deformed bubble
is different from the direction of the streamlines, and is distributed asymmetrically with respect to the
lateral(horizontal) plane that penetrates the sphere center. Thus, the individual bubble has a transient
deformation and does not reach steady deformation at any point in the flow field while the liquid flow
field itself is steady. In other words, the individual bubble experiences a temporal change in shear rate
when it moves relative to the sphere. This is why falling sphere viscometry can assess the influence of
transient bubble deformation.
The physical mechanism behind the effect of bubbles’ elasticity, i.e. transient bubble deformation,
should be investigated further. Mathematical explanation can be deduced with the idea of so-called
574 Y. Murai, H. Oiwa / Fluid Dynamics Research 40 (2008) 565 – 575

Fig. 6. Bubble deformation pattern around falling sphere.

complex viscosity that arises when the elastic and the viscous stresses take place accompanying a phase
lag. Experimental approach by measuring the local liquid behavior among in-deforming bubbles is also
expected to characterize this phenomenon comprehensively.

4. Summary

Falling sphere viscometry, i.e. the measurement of the viscosity of fluids via the terminal velocity of a
sphere in a Stokes drag region, reveals that the effective viscosity increases significantly in bubbly liquids
when individual bubbles have transient deformation. While the Stokes flow field is steady, bubbles are
subjected to an unsteady shear rate during their motion relative to the sphere. This approach successfully
assesses the effect of unsteady bubble deformation. For low capillary numbers, the measurement results
for relative viscosity matches the Stokes–Einstein viscosity;  = 1 + . Bubbles for high Ca numbers have
the relationship  =1−(5/3). The critical Ca number, which is defined when the viscosity is unaffected by
bubbles, i.e. =1, is obtained to be Ca=3.3. This critical Ca number is found to be much larger than that for
steady bubble deformation; Ca=0.65. Thus during stretching, bubbles provide significant additional shear
stress to the layer around the sphere, and increase the drag to slow down the settling velocity. This phe-
nomenon is ignored in current computational models of bubbly flow, however, the authors think that bub-
bles’ transient deformation considerably alters the local shear event in bubbly liquid that is subjected to un-
steady
flow.

Acknowledgments

This research is supported by a grant-in-aid scientific research from the Japanese Society for Promo-
tion of Science (No. 17686014). The authors also express their thanks to Prof. S. Fujikawa (Hokkaido
University, Japan) and Prof. A. Prosperetti (Jhons Hopkins University, USA) for their advice on this
topic.
 Y. Murai, H. Oiwa / Fluid Dynamics Research 40 (2008) 565 – 575 575

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