Chemical Engineering Science 59 (2004) 3793 – 3805

www.elsevier.com/locate/ces

Mixing analysis in a tank stirred with Ekato IntermigJ impellers

E.S. Szalaia , P. Arratiaa , K. Johnsonb , F.J. Muzzioa;∗
a Department of Chemical and Biochemical Engineering, Rutgers University, 98 Brett Road, Piscataway NJ 08854-8058, USA
b Independent Consultant, 2884 Sutherland Circle NW, North Canton, OH 44720, USA

Received 4 October 2002; received in revised form 14 November 2003; accepted 1 December 2003

Abstract

The mixing performance of a batch stirred tank with four Ekato IntermigJ impellers is investigated in this paper by experimental
and computational methods. We considered three impeller speeds corresponding to Reynolds numbers 37, 50 and 100, all in the laminar
regime. For the purposes of model development and 9ow validation, Newtonian rheology is assumed, where the 9uid density and viscosity
is set to 1247:6 kg=m3 and 0:4 kg=(m s), respectively. The computed velocity ;eld and mixing patterns are validated using Particle Image
Velocimetry, acid-base visualization experiments and Planar Laser-Induced Fluorescence. All three techniques reveal excellent agreements
between the experiments and computations. Also, detailed Lagrangian analysis of mixing, using particle tracking and stretching simulations,
is presented for two 9owrates in the laminar regime. It is shown that severe compartmentalization exists in the vessel and transport in the
axial direction is very slow. Characterization of local micromixing intensities is presented by computing the distribution of intermaterial
area density and striation thickness distribution (STD) from the stretching ;eld. It is found that the STDs at both 9owrates are identical
despite signi;cant di@erences in the stretching ;eld, suggesting that at low stirring rates micromixing performance is independent of
agitation speed.
? 2004 Published by Elsevier Ltd.

Keywords: Mixing; Fluid mechanics; Microstructure; Homogenisation; Numerical analysis; Visualization

1. Introduction 9ow behavior often causes a decrease in productivity. The

One of the most challenging tasks in the chemical, phar-
maceutical and biochemical industry is the design and
scale-up of reactors, when highly viscous 9uids are pro-
cessed. Commercial applications include antibiotic and
polysaccharide fermentations, vaccine and glycoprotein
production, or distributing additives in creams, pastes and
paint. The formation of persistent slow-mixing regions at
low impeller speed, or the diBculty of handling materials
with complex rheological behavior often excludes most tra-
ditional scale-up methods from the list of engineering tools
designers can use. Handling highly viscous 9uids presents
an interesting problem from a mixing viewpoint, because
poor bulk mixing, low oxygen mass transfer rates, and in-
homogeneous distribution of substrate are inherent in these
applications. While the intrinsic rate of biological reactions
remains virtually independent of vessel size, the hydro-
dynamic environment changes upon scale-up. Non-ideal
∗ Corresponding author. Tel.: +1-732-445-3357; fax: +1-732-445-
6758.
E-mail address: muzzio@soemail.rutgers.edu (F.J. Muzzio).
degree of agitation at all levels must be suBcient to elimi-
nate dead zones, which could become anaerobic, break up
and distribute air bubbles from the sparger and accomplish
satisfactory bulk mass and heat transfer. Which one of these
processes becomes the most outstanding challenge usually
depends on the scale of the operation, the exact rheological
properties of the broth and the sensitivity of the microor-
ganisms to shear and oxygen levels.
The mixing performance of stirred tanks equipped with
various types of agitators, such as Rushton or piched-blade
turbines, has been considered by many researchers (Nienow
and Elson, 1988; Nienow, 1990; Amanullah et al., 1998,
2001). Recently high 9ow and low power number impellers,
such as the Intermig and axial hydrofoil impellers, have
became prevalent (Galindo and Nienow, 1992; Bujalski
et al., 1999; Ibrahim and Nienow, 1999; Houcine et al.,
2000). Most investigations have examined the mixing time
and power consumption of agitation systems resulting in
highly speci;c empirical correlations (Mavros et al., 1996;
Rutherford et al., 1996; Esponosa-Solares et al., 1997;
Armemante and Chang, 1998), but the micromixing prop-
erties of most impeller types have not been considered.

0009-2509/$ - see front matter ? 2004 Published by Elsevier Ltd.

doi:10.1016/j.ces.2003.12.033
3794 E.S. Szalai et al. / Chemical Engineering Science 59 (2004) 3793 – 3805
In this paper we focus on the performance of the Ekato
Intermig impellers, considering both the 9ow and mixing
properties of these low-shear agitators. These impellers are
usually installed in pairs, with each agitator rotated at a
90◦ angle with respect to its neighbors. The two pumping
directions of the center and head portions of the Intermig
is signi;cant for oxygen distribution, but 9ooding occurs
more often at a particular aeration rate if the center impeller
pumps downwards (Nienow, 1990). It is suggested that the
Intermigs produce a complex 9ow pattern that bears little re-
semblance to the simpli;ed version given by manufacturers
(Ibrahim and Nienow, 1995). In this paper we examine the
performance of a fermenter equipped with four Ekato Inter-
migs by experimental and computational techniques. These
methods and the exact geometry is described in Section 2.
A detailed analysis of the 9ow ;eld and mixing patterns un-
der laminar conditions is provided in Section 3. In this sec-
tion we also compute mixing intensity based on stretching
computations (Muzzio and Swanson, 1991) and discuss a
quantitative measure for micromixing eBciency.
2. Geometry and methods
Flow and mixing is investigated in a stirred tank geometry
that is commonly used as a reactor, fermenter or crystallizer.
In order to analyze the hydrodynamical environment and
mixing performance in the tank by experimental methods,
a laboratory-scale vessel is built from plexiglass according
to the dimensions in Fig. 1(a). An identical computational
model of the geometry is created using the ORCA CFDJ
software package (Dantec Dynamics, Mahwah, NJ), which
consists of 3.7 million tetrahedral volume elements and 1.1
million nodes. The tank diameter, T is set to 0:3048 m and
the height to diameter ratio (H=T ) is 2.75. The vessel is
agitated by four Ekato IntermigJ impellers, which are con-
structed following the manufacturer’s standards. For an en-
larged view, see Fig. 1(b). This type of impeller is usually
installed in pairs, where each one is rotated 90◦ relative to
its neighbors. The schematic drawing indicates the position
of four impellers, spaced at equal distances (7 apart) from
one another and the tank bottom. Subsequently, we number
each impeller as #1 starting at the tank bottom to #4 at the
top. The round bottom of the vessel was simulated as an el-
lipse, where the radius of the major axis is the tank radius
(equal to 6 ) and the radius of the minor axis is 2 .
Flow in stirred tanks is generally characterized by the
Reynolds number (Re), de;ned as follows:
ND2
Re = ; (1)
where N is the impeller speed in revolutions/s, D is the
impeller diameter,  is the 9uid density in kg=m3 and  is
the 9uid viscosity in kg=(m s). Three 9ow conditions are
examined in this investigation, Re = 37, 50 and 100, all in
the laminar regime. For the purposes of model development
and 9ow validation, Newtonian rheology is assumed in this
work. The 9uid density and viscosity is set to 1247:6 kg=m3
and 0:4 kg=(m s), respectively. These values are similar to
the physical properties of a glycerine-water mixture at room
temperature. No-slip boundary conditions were assumed for
the simulations for all 9uid–solid interfaces. The vessel is
open to the atmosphere at the top 9uid–9uid interface, so a
zero stress boundary condition was applied to that surface.
2.1. Solver technology and computational methods
The ORCA CFDJ package is used in the computational
analysis of 9ow and mixing behavior. Details of the compu-
tational methods are given elsewhere (Shakib et al., 1991;
Szalai and Muzzio, 2003; Zalc et al., 2002). Only a brief
summary is included here for the sake of brevity. The model
of the Intermig impeller geometry is custom-built, accord-
ing to the exact speci;cations by Ekato, and assembled in
a CAD-type modular unit to facilitate user-friendly appli-
cations. Numerical solutions for the coupled velocity and
pressure ;eld are computed at the 1.4 million nodal loca-
tions in the three dimensional (3D), unstructured mesh of
the geometry. The solver technology in the ORCA pack-
age is based on a stable iterative method with Galerkin
;nite-element formulations. Similarly to other CFD solvers,
it requires a maximum convergence tolerance and forces
the di@erence between successive iterations below the pre-
set limit. In the present analysis, the steady-state 9ow solu-
tions converged below the 10−4 tolerance in seven iterative
steps in the four-impeller vessel. The divergence-free con-
straint of time-independent 9ows was enforced for all three
9owrates. The total memory requirement for each solution
was 1:36 Mbytes on a single workstation (Sun Solaris ul-
tra60 processor).
The nodal values of velocity and pressure ;eld serve as
the starting point for mixing analysis by Lagrangian parti-
cle tracking calculations. Particle trajectories are integrated
via a fourth order, adaptive step-size routine following the
velocity vector ;eld:
dx
= v(x):
N (2)
dt
Mixing processes promote contact between mixture compo-
nents, which means increasing the interfacial area available
for transport of mass and energy and decreasing di@usional
distances between various species. The increase in interfa-
cial area that occurs as a result of the mixing process is mea-
sured by the elongation of small vectors attached to 9uid
particles (i.e. stretching) as they move through the 9ow. The
evolution and statistics of stretching in chaotic 9ows has
been exploited in detail (Ottino, 1980; Muzzio and Swanson,
1991; Beigie et al., 1993; Liu et al., 1994), and some rela-
tionships are summarized brie9y here. The elongation of an
in;nitesimal vector l with initial length l0 attached to each
 E.S. Szalai et al. / Chemical Engineering Science 59 (2004) 3793 – 3805 3795

Fig. 1. (a) The geometry of a tank stirred with four Ekato Intermig impellers. (b) An Ekato Intermig impeller. (c) Experimental velocity ;eld in the
tank, measured by Particle Image Velocimetry, in the region marked by the red box in (a). (d) The simulated 9ow ;eld is shown in the same region
for comparison.

9uid particle is computed by integrating (3):
dl
= (∇v)T · l (with the initial condition lt=0 = l0 ):
dt
The overall length increase, or accumulated stretching (e.g.
strain), for a given particle trajectory is de;ned as
distributing a collection of vectors in the 9ow (as opposed
to a single vector) and measuring a ;eld of stretching in-
tensities as a function of position and time. The distribution
(3)
of stretching intensities generated by the 9ow then provides
a quantitative assessment of mixing performance. The fre-
quency of  values can be computed as

|l| 1 d N (log )
= : (4) H (log ) = ; (5)
|l0 | N d log 

Since the rate of accumulation of  is exponential, the evolu-
tion of the stretching in chaotic 9ows can be best described
using a logarithmic scale.
Quantifying the eBciency of a mixing process requires
resolving the emerging spatial structure of the mixture by
where N is the total number of vectors used to compute the
stretching ;eld. The base 10 logarithm of  is adapted for
all results discussed in this paper.
Being able to measure and predict the rate of growth
of interface and its area coverage, or intermaterial area
3796 E.S. Szalai et al. / Chemical Engineering Science 59 (2004) 3793 – 3805
density, , is an important step towards understanding re-
active processes. Intimate contact between mixture compo-
nents is necessary for chemical reactions and assures high
local rates of mass transfer. The spatial distribution of inter-
material area is unique in every chaotic 9ow. However, in
all chaotic 9ows the interface grows exponentially:  ≈
en . Here  represents the topological entropy of the 9ow,
which is the true “mixing rate” in the system, and n is the
period (n = 2 for one impeller revolution, when using In-
termigs). With the relationship =∼= (Muzzio et al.,
2000), the spatial distribution of intermaterial contact area,
scaled by the overall length of the interface , can be pre-
dicted directly from the stretching ;eld in a mixer:
H (log ) H (log ) 1 dN (log )
= = : (6)
  NP  d log 
The stretching ;eld can be formally related to the stria-
tion thickness distribution (STD) in chaotic 9ows. Material
;laments are stretched in one direction and simultaneously
compressed in another direction at the same rate, the striation
thickness is directly related to the stretching of a material
;lament: s∼1=∼1=. As a consequence of this relationship,
the time evolution, shape, and scaling of stretching distri-
butions in globally chaotic 9ows is also related to the same
properties of striation thickness distributions. Because new
striations are born in a chaotic 9ow after every passing of
the impeller, there is a proportionality, the intermaterial area
density (), that links the stretching ;eld with the number of
striations. Considering that the number of stretching values
is constant at each 9ow period, while the number of stri-
ations increases (i.e. (Ns )∼), the striation thickness
distribution, as predicted from the stretching ;eld, follows:

H (log s) = H (log ): (7)

The real power of this relationship is that while H (log s)
is unattainable directly in most 9ows, computing H (log )
is fairly straight-forward. It is shown in this paper that the
STD can be predicted in complex 3D 9ows based on the
stretching ;eld and Eq. (7).
2.2. Experimental methods
The computational techniques used in this study do not
require any experimental input for a 9ow solution, but it is
always necessary to validate the numerical results. For that
purpose, three non-intrusive optical techniques, Particle Im-
age Velocimetry (PIV), acid-base 9ow visualization exper-
iments and Planar Laser-Induced Fluorescence (PLIF) are
used to measure the experimental 9ow patterns and compare
with the numerical solutions.
PIV yields velocity vectors at multiple locations with a
single experiment. It determines the linear displacement of
particles suspended in the 9ow. After seeding the 9uid with
tracer particles, a laser is used to illuminate a cross-section of
the 9ow and two pictures are taken in a short time. Knowing
the time interval between the two pictures and the distance
particles moved yields velocity information at all the particle
locations simultaneously along the planar cross section. In
the validation studies this technique was primarily used to
measure velocity 9ow ;elds which were then compared to
9ow ;elds calculated by CFD.
PLIF is an instantaneous, whole-;eld measurement tech-
nique, where a 9uorescent dye in solution with one of the
mixture components is excited with laser light. It reveals
the evolution of mixing patterns by dispersing a 9uores-
cent tracer 9uid in the system. Flow and mixing behavior,
concentration ;eld, and reaction rate information can be
measured from the intensity of 9uorescence between the
mixture components. A small amount of 9uorescent dye
(Rhodamine) is injected to the tank and illuminated with a
laser light in the experiments. The spreading of the dye is
followed in the 9ow by taking a series of pictures, and the
concentration is quanti;ed based on the intensity of 9uo-
rescence. Experimental pictures are taken at various cross
sections in two dimensions, because folds and layers of the
illuminated tracer 9uid at di@erent depths in the evolving
mixing structure would overlap in a 3D view and hide ;ne
details.
A third experimental method, a visualization technique
based on an acid-base neutralization reaction was also used
to exploit the size and shape of segregated regions in the
mixing tank. This technique is based on adding a soluble,
pH sensitive indicator to the 9uids to be mixed. The indica-
tor appears blue in basic environment and yellow in acidic
media. When the mixture components come in contact dur-
ing the mixing process, the neutralization reaction instanta-
neously proceeds at the interface and a color change occurs.
In slow-mixing regions, or islands, the 9uid appears blue for
long times, because there is not enough acidic component
for complete neutralization. The reaction rate is limited there
by the very slow rate of di@usive transport mechanisms.
3. Results
3.1. Flow patterns and experimental validation
Fig. 1(c) and (d) shows the comparison of the com-
puted and experimentally measured 9ow ;eld at Re = 37.
The experimental velocity vectors were measured in a plane
aligned with one of the impeller blades using PIV and col-
ored by increasing magnitude from dark blue to yellow. In
order to illustrate the agreement between the computed and
experimental 9ow patterns, a section of the mixing vessel
framed by a red box in Fig. 1 is enlarged for visual clar-
ity. The velocity measurements indicate that a complex, 3D
9ow pattern forms in the vessel that creates strong varia-
tions in the azimuthal direction, so phase locking between
the experimental and computational measurements is criti-
cal. Fluid motion is dominated by 9ow created at the tip of
each impeller blade. The tip of the ;rst impeller creates a
strong axial 9ow, moving 9uid toward the second impeller.
An S shape bulk pattern is observed between these two
 E.S. Szalai et al. / Chemical Engineering Science 59 (2004) 3793 – 3805
Fig. 2. The probability density function of the velocity is computed from
the experimentally measured and the simulated 9ow ;eld. The statistical
comparison is excellent in both (a) the X direction and (b) the Y direction.
impellers, as the 9uid reaches wake of the second impeller
and is ejected toward the wall by the strong radial 9ow in
that region. A recirculation loop just below the plane of the
second impeller is seen in this section. Overall, the computed
result compares well with the experimentally measured 9ow
despite the complexity of the convective motion created by
the impellers in this section. Surprisingly, the long, pitched
blades closer to the hub has minimal e@ect on axial 9ow and
mixing in the vessel. Our observation, that much stronger
radial, rather than axial 9ow is created by each impeller, is
consistent with results of other investigations ( Ibrahim and
Nienow, 1995) concluding that a strong radial 9ow develops
with a small downward discharge angle below Re = 170.
A quantitative comparison of the experimental and com-
putational velocity ;elds can be made by computing the
probability density function (pdf) of the velocity compo-
nents vX and vY :


1 dN (va )
pdf (va ) = ; (8)
Np dva
where dN (va ) is the number of vectors that have veloc-
ity values between va and (va + dva ). The parameter ‘a’ in
Eq. (8) represents x or y, and Np is the total number of ve-
locity vectors. The physical meaning of pdf (va ) is the rel-
ative distribution of velocities from smallest to largest val-
ues at a selected location. Fig. 2 shows the pdf (vX ) and
the pdf (vY ) at a vertical cross-sectional plane in the tank
aligned with two of the impeller blades. The most important
3797
Fig. 3. The velocity ;eld, measured in a cross-sectional plane aligned with
two of the impeller blades, is color-coded by magnitude (a) at Re = 50
and (b) at 100 in the tank.
information in Fig. 2 is that the accuracy of the computed
velocity values (red) is reasonable compared to the experi-
mental measurements (black) for both the x (Fig. 2(a)) and
y component (Fig. 2(b)) despite the complex 9ow pattern.
This comparison establishes a high level of con;dence in the
computational methods and these techniques in turn can be
used to describe experimentally unattainable characteristics
of the mixing process.
The computational velocity ;eld for two 9owrates, Re=50
and 100, is shown in Fig. 3. Each ;gure shows half of the
tank cross section, where the shaft is on the left and two
of the impellers are aligned with the vertical cross-sectional
view. The impeller hubs are shown to mark the location of
all four impellers. There are large variations from low to
high velocities in the 9ow and a non-intuitive 9ow pattern
is revealed in the tank cross-section. Several recirculation
loops exist in the vessel, one above and one below each im-
peller blade. A large recirculation loop ;lls the bottom por-
tion of the tank. Fluid in this region passes through impeller
#1, it is pushed towards the vessel wall and returns towards
the shaft.
Above each impeller aligned with the vessel cross-section
strong axial 9ow is created towards the tank top, forming an
S shape bulk 9ow pattern. As the impeller passes through the
3798 E.S. Szalai et al. / Chemical Engineering Science 59 (2004) 3793 – 3805

plane, the 9ow direction reverses in the same region towards

the bottom of the vessel. This behavior is also observed as
the Re number is increased to 100 (Fig. 3(b)). The overall
9ow pattern is almost identical to the one at Re = 50, but
more intense gradients are apparent at the higher Re number
case, due to the increased amount of inertia at the larger
agitation rate.
After establishing a high level of con;dence in the com-
putational techniques, the following sections focus on the
evolution of mixing structures. Because the 9ow ;eld is
fully 3D, it is inappropriate to conclude that the recircula-
tion loops represent segregated regions in the tank without
performing a Lagrangian mixing analysis.

3.2. Short-term mixing structures

Recently, it has been shown that the chaotic mixing pro-

cess in stirred tanks is driven by small 9ow perturbations
caused by the passing of the impeller blades (Zalc et al.,
2002). In fact, no laminar mixing is possible if the impeller
blades are removed and replaced by concentric disks, be-
cause at low Reynolds numbers the 9ow is steady and 2D.
In such 9ows, particle trajectories follow closed streamlines
and simply trace out nested tori. There is no convective
exchange of material among these tori, hence mixing can
occur only by slow di@usive transport. When 9uid is agi-
tated by impellers, the passage of 9uid elements through the
near-blade regions brings about stretching and reorientation.
The 9uid elements must move towards the wall to allow
for the passing of the impeller blades. This mechanism of
stretching and reorientation is illustrated by the computed
short-term mixing structures in Fig. 4.
Since particles located near the shaft tend to be ejected
outward radially by the impellers, 200,000 tracer particles
are injected initially along the shaft in a vertical line extend-
ing along the height of the tank. Radial mixing e@ects are
most noticeable because tracer particles are initially placed
in regions where they quickly pass through the blade section
of the impellers. When distributing additives, this region is
best for injections. The position of particles is recorded after
every 10 impeller revolutions (20 9ow periods). The com-
puted mixing structures at Re = 50 are shown in Figs. 4(a)
and (b) after 10 and 20 revolutions, respectively. Fluid tracer
particles initially injected in the top half of the vessel are
colored red and tracers initially placed in the bottom half are
colored blue in the ;gure. In Fig. 4(a) particles are ejected
along the center of each impeller towards the tank wall and
then invade the top and bottom section of the compartments
surrounding each impeller. As particles reach the tank wall,
the stream splits and feeds the top and bottom part of each
chamber returning toward the shaft to be re-injected along
the centerline again.
Severe axial mixing limitations are immediately apparent
from the mixing patterns at Re = 50 in Figs. 4(a) and (b).
The e@ect of poor axial mixing is revealed by the complete
Fig. 4. The mixing structure after (a) 10 and (b) 20 impeller revolutions
at Re = 50.
segregation of the red and blue colored tracer 9uid in the
top and the bottom of the tank, respectively. Red tracer 9uid
was injected only in the top region and it remains there
after 10 impeller revolutions (Fig. 4(a)). As the impellers
rotate for another 10 revolutions, more 9uid striations are
created around the blades, but the axial mixing barrier at the
mid-height of the tank is not penetrated.
The e@ect of poor axial mixing persistently remains as the
agitation speed is increased to Re=100 in Figs. 5(a) and (b).
The computed mixing patterns after 20 and 40 impeller rev-
olutions are shown at the higher agitation rate corresponding
to 42 RPM. Fluid tracer particles are color-coded similarly
to the Re = 50 case (tracer particles initially injected in the
top half of the vessel are colored red and tracers initially
placed in the bottom half are blue in the ;gure). The two
9uids remain almost completely segregated as they spread
throughout the chambers around each impeller. In Fig. 5(a),
no red dye visits the bottom half of the vessel and conversely
no blue dye enters the top region. After 20 revolutions some
particles are entrained along the shaft, but there is essen-
tially no convective mixing across the separation plane at the
mid-height of the tank. Such severe compartmentalization in
the 9ow can cause signi;cant mixing limitations. Transport
across this permanent boundary only occurs via di@usion,
which is generally too slow to assure complete homogeneity
 E.S. Szalai et al. / Chemical Engineering Science 59 (2004) 3793 – 3805
Fig. 5. The mixing structure after (a) 20 and (b) 40 impeller revolutions
at Re = 100.
in most practical applications. As a consequence, large vari-
ations in yield or 9uctuations in eSuent product and/or waste
concentrations may be observed. Moving towards the top of
the vessel, some very small segregated regions are also no-
ticeable along the shaft. Due to their small size, these islands
do not signi;cantly a@ect mixing performance.
The mixing patterns in Figs. 4 and 5 reveal that a pro-
nounced structure of lobes is created as a result of the peri-
odic stretching and folding caused by the impellers. These
lobes gradually wrap around a slow-mixing region at the
center of each chamber. The overall appearance of the mix-
ing pattern from 10 to 20 revolutions (Figs. 4(a) and (b))
remains similar, only more folds appear in fast-mixing areas.
Self-similarity, the evolution of mixing patterns towards an
asymptotic structure, is characteristic of all periodic chaotic
9ows. An underlying ;eld of orientations controls the struc-
ture of 9uid striations at each location in the 9ow. The orien-
tation process, controlled by a property named Asymptotic
Directionality, is very fast and the dependence on initial in-
jection location is lost exponentially fast (Giona et al., 1998;
Muzzio et al., 2000).
Recirculating regions create multiple slow-mixing regions
in the 9ow above and below each impeller. Figs. 4(b) and
5(a) reveal the e@ect of these slow-mixing regions, where
3799
mixing patterns after 20 revolutions can be compared for
two agitation rates, Re = 50 and 100, respectively. Examine
the region below impeller #1, where a large recirculation
loop forms a slow-mixing region. The short-time evolution
of the mixing patterns indicate that even though segregated
regions are small after long times, the 9uid surrounding
these regions mixes at a very slow rate. Colored 9uid tracer
particles invade the star-shaped islands very slowly and this
e@ect increases at larger rates of agitation. The size of the
slow-mixing region devoid of dye in Fig. 4(b) after 20 rev-
olutions is signi;cantly smaller than in 5(a) after the same
number of impeller rotations. However, 20 revolutions at
Re = 100 corresponds to half of the processing time as for
Re = 50. Figs. 4(b) and 5(b) indicate mixing after the same
amount of time (1 min) for the two agitation rates. The same
observation can be made about the e@ect of the slow-mixing
regions as before: mixing in the Re = 100 case is a@ected
more signi;cantly. The size of the unmixed region in 5(b)
is approximately double compared to 4(b).
An acid-base visualization experiment, as described in
Section 2, was carried out to con;rm the computational mix-
ing analysis and examine axial mixing in the tank. Figs. 6(a)
–(f) shows a series of experimental photographs, where the
tank is originally ;lled with a viscous glycerine-water mix-
ture that contains NaOH base and Bromothymol blue pH
indicator. The impeller speed in these experiments corre-
sponds to 21 RPM, the same as in Figs. 4(a) and (b). The
entire vessel initially appears blue, because the pH is slightly
above 7. A small amount of acidic 9uid is then injected
near the top of the vessel at the start of the experiment. As
the mixing process evolves and the two 9uids come to in-
timate contact, the neutralization reaction changes the pH.
Thus, the 9uid appears yellow in all well-mixed areas, and
remains blue in regions where acidic 9uid is yet not trans-
ported. Fig. 6(a) reveals that acidic 9uid invades the cham-
ber around the top impeller and indicates the location of the
separation plane and the doughnut-shaped, slow-mixing re-
gions above and below the impeller. After 15 min Fig. 6(c),
the top compartment is almost completely mixed, but only a
very small amount of acidic 9uid gets to the region around
the second impeller from the top. In an additional 15 min
most of the top half of the vessel is well-mixed, except for
two slow-mixing regions around the second impeller. After
90 min the slow-mixing regions in the top are almost com-
pletely destroyed, but there is a clear boundary to convective
transport between the top two and the bottom two impellers.
A small discoloration of the third chamber from the top in-
dicates that some 9uid is slowly transported to the bottom
along the shaft, which is consistent with the results of the
computations in Fig. 4. Clearly, there is a severe limitation
in axial mixing, despite indications of axial 9ow created by
the Intermig impellers.
Almost all mixing tanks are designed with the shaft
placed at the center of the vessel and agitators usually have a
plane of symmetry. The symmetric con;guration is the least
e@ective from a theoretical standpoint, because it promotes
3800 E.S. Szalai et al. / Chemical Engineering Science 59 (2004) 3793 – 3805

Fig. 6. Mixing patterns captured by an acid-base experiment using constant agitation speed at Re = 37.

Fig. 7. Mixing patterns captured by an acid-base experiment using variable agitation speed.

segregation and creates time-periodic conditions. One ap-
proach to overcome the limitations of such geometries
is to vary the speed of the impellers. It has been shown
that systematically alternating the agitation rate destroys
slow-mixing regions below and above a single Rushton
impeller (Lamberto et al., 1996). In this paper this tech-
nique is applied to perturb the separation plane at the
mid-height of the vessel and promote rapid and eBcient
mixing. The results of variable speed agitation carried out
in the tank with Intermig impellers is indicated in Fig. 7,
where Figs. 7(a)–(d) shows a series of photographs as
the agitation rate is alternated between 21 and 42 RPM
every 1 min. Similarly to the previous experiment shown
in Fig. 6, the tank is initially ;lled with a mixture of glyc-
erine and water containing base and bromothymol blue
pH indicator. After the acidic 9uid is injected near the
top, the impeller speed is systematically increased and de-
creased every 5 min. Using the variable speed technique,
the top-bottom segregation at the center of the tank is
completely eliminated in 30 min (Fig. 7(d)). In contrast to
Fig. 6(d), where top to bottom segregation persists after
90 min when the agitator speed is constant, Fig. 7 indicates
 E.S. Szalai et al. / Chemical Engineering Science 59 (2004) 3793 – 3805
Fig. 8. Comparison of (a) PLIF and (b) computed 9ow structures below an Intermig impeller.
that the variable speed technique e@ectively destroys axial
segregation.
Next, the mixing behavior in a small section of the tank
is examined in detail. A very complex, ;lamented mix-
ing structure is created by the impellers. The details of the
mixing pattern around one of the impellers is enlarged in
Figs. 8(a) and (b). The experimental mixing pattern in Fig.
8(a) is captured by LIF measurements, described earlier in
Section 2. In these experiments 9uorescent rhodamine dye
is injected initially at the tip of the impeller blades and a
laser is used to illuminate a cross-section of the vessel near
the center. As mixing proceeds, a series of pictures are taken
by a CCD camera. Well-mixed areas appear yellow and the
intensity of 9uorescence is an indication of mixing inten-
sity in each region of the 9ow. The computational mixing
pattern in Fig. 8(b) appears almost identical to the experi-
mental mixing structure. Hence, the physics of 9uid motion
is captured correctly in the computational model. Addition-
ally, both pictures reveal the formation of lobes near the tip
of the impeller that travel towards the tank wall and then
wrap around the slow-mixing region below the impeller. The
periodic passing of the impeller blades creates new folds
each time and the 9ow stretches and folds the already exist-
ing ones. A similar mixing mechanism has been observed
when using Rushton impellers (Zalc et al., 2002), where the
perturbations created by the Rushton impeller blades were
signi;cantly smaller in size. These folds are created as the
impeller blades periodically increase the intermaterial con-
tact area between two 9uids. The more ;lamented the struc-
ture, the more area is available for di@usion to occur and
ultimately complete the homogenization on the micromix-
ing scale. The folds created by the Intermigs invade a larger
region of the 9ow compared to other impeller types such
as the Rushton or the pitched-blade (Lamberto et al., 1999;
Alvarez et al., 2002).
3.3. The stretching :eld
The ultimate goal of a mixing application is to increase the
intimacy of contact between mixture components and create
3801
suBcient area for di@usional transport. As 9uid ;laments
are stretched and folded by the 9ow, they gradually deform,
increase in length and simultaneously decrease in width.
The length increase which the 9uid ;laments experience
can be measured by stretching computations. The stretching
;eld captures the increase in the contact area between 9uid
;laments during the mixing process (Muzzio and Swanson,
1991; Szalai and Muzzio, 2003).
The stretching of material ;laments was computed in the
tank by placing 200,000 small vectors in the 9ow and inte-
grating Eqs. (2) and (3) simultaneously. Fig. 9 shows the
stretching ;eld in the tank at Re = 50. The colors from blue
to red represent the logarithm of the stretching as a function
of initial position, from low to high intensities. After 10 rev-
olutions in (a), a complex, highly inhomogeneous stretching
;eld emerges. The slow-mixing regions observed in the mix-
ing patterns (Fig. 4) coincide with the blue, low-stretching
regions in Fig. 9(a). It is important to note that the color as-
signment is based on a logarithmic scale, so there is multiple
orders of magnitude di@erence between the high stretching
(red) and low stretching (blue) regions. A very inhomo-
geneous intensity ;eld is not bene;cial for shear-sensitive
materials, such as mammalian cell cultures. As cells visit
di@erent regions of the 9ow, they experience orders of
magnitude changes in shear and can su@er signi;cant
damage.
The stretching ;eld for Re = 100 is shown in Fig. 9(b).
Although the distribution of high- and low-intensity regions
is somewhat di@erent for this 9owrate than for Re=50, some
important characteristics remain unchanged. The stretching
;eld in Fig. 9(b) is also very inhomogeneous, and high-shear
regions appear at the plane of every impeller and at the
mid-plane between each blade. The ;eld of mixing inten-
sities measured by stretching represents the micromixing
properties of the 9ow for the duration of the mixing process.
The spatial inhomogeneities remain unchanged and do not
disappear over time. As shown in Figs. 4 and 5, a character-
istic property of chaotic 9ows is that contact area between
mixture components always accumulates at the same spa-
tial locations. Because there is an invariant ;eld of orien-
tations dictating how 9uid striations form and orient in the
3802 E.S. Szalai et al. / Chemical Engineering Science 59 (2004) 3793 – 3805

Fig. 9. The stretching ;eld (), color-coded by the magnitude of the ac-
cumulated stretching on a logarithmic scale, is shown after 20 revolutions
(a) at Re = 50 and (b) at Re = 100.

9ow, the intensity ;eld as well as the mixing patterns re-

main self-similar. Thus, it is suBcient to describe the local
mixing intensities at one instant in time to fully characterize
the entire mixing process.
This information can be used to identify areas in the tank
with high local intensity of mixing. In other words, e@ective
injection locations can be identi;ed by the high-stretching,
red areas in the tank. For instance, if a small amount of ad-
ditive needs to be distributed relatively fast in the mixing
vessel, areas near the tip of each blade are recommended
for eBcient mixing. Blue, low-stretching areas are very
slow-mixing regions, as seen earlier in the mixing patterns
in Figs. 4 and 5. If nutrients are added here for distribu-
tion, they remain trapped inside these regions for long times.
Only di@usion transports material from these low stretching
regions to the bulk 9uid.
It is instructive to look at the distribution of mixing in-
tensities in a quantitative manner by computing the pdf of
the natural logarithm of the stretching values, H (log()):


1 dN (log )
H (log ) = ; (9)
Np d log 
where dN (log()) is the number of vectors that have stretch-
ing values between log() and log() + d log() and Np
Fig. 10. The logarithm of the probability density function of log(),
(log(H (log())), at (a) Re = 50 and (b) at Re = 100.
is the total number of stretch vectors. In physical terms,
Hn (log()) represents the spectrum of intensities in the mi-
cromixing process. Fig. 10(a) shows plots of log(H (log()))
versus log() for the Re=50 9ow after 10, 20, 30, 40, 50 and
60 impeller revolutions. The distribution curves shift toward
higher stretching values as the total number of revolutions
increases. As stretching accumulates, the curves broaden,
but retain a constant shape.
Fig. 10(b) shows similar results for Re =100. In all cases,
the distributions exhibit multiple peaks (with mean values in
the low and high stretching regions). The distinct peaks near
log()–0 for each Re number represent the stretching expe-
rienced by ;laments initially placed within the segregated
 E.S. Szalai et al. / Chemical Engineering Science 59 (2004) 3793 – 3805
regions in the 9ow. These peaks of low stretching values
remain virtually ;xed as the number of impeller revolutions
increases, because the stretching inside slow-mixing islands
increases at a slow linear rate, if at all.
3.4. Micromixing intensities
The thickness of 9uid ;laments is the most fundamental
measure of the di@usive length scale in the mixture. This
is the distance 9uid molecules must ultimately travel to
complete the homogenization process. However, this mea-
sure of local micromixing intensity cannot be assessed by
experimental techniques, because the average thickness of
9uid striations rapidly decreases below micron size in the
course of a mixing process. The average length scale rapidly
falls below experimental resolution in complex 9ows. The
scaling properties of stretching discussed above can be ex-
tended to generate useful predictions of micromixing in-
timacy, and compute the striation thickness. Clearly, the
same iterative stretching-and-folding process that generates
self-similar stretching distributions drives the evolution of
striations, and therefore controls the dynamics of Striation
Thickness Distributions (STDs).
STDs could be computed directly from distributions of
stretching values by realizing that as a portion of 9uid is
stretched, it generates striations with a thickness (s) in-
versely proportional to the amount of stretching () applied
to the 9uid (Muzzio and Swanson, 1991). Moreover, the
number of such striations in a portion of 9uid (dN (s)), which
is proportional to the amount of contact area , is also pro-
portional to the stretching:
s∼1=; (10a)
ds∼ − 2 dN (); (10b)
dN (s)∼ − dN (); (10c)
where the minus sign in Eq. (10c) re9ects that a list or-
dered in increasing magnitude of s results in a list ordered
in decreasing order of . Eq. (10) can be simply re-stated
in terms of the logarithms of s and  as
d(log s)∼ − d(log ); (11a)
dN (log s)∼ − dN (log ): (11b)
Finally, one needs to take into account the fact that while
the number of stretching values remains constant with n, the
number of striations, Ns , increases as
Ns ∼∼: (12)
In principle, Eqs. (11) and (12) are everything one needs to
predict the striation thickness distribution:
1 dN (log s) 1  d N log )
H (log s) = ∼ demonstrates that the overwhelming majority of striations,
Ns d(log s)  d(log )
 tank, is generated by a set of very rare, but very intense
= H (log ): (13)

3803
The validity of Eq. (13) was demonstrated recently (Alvarez
et al., 1998), where the micromixing structure H (log s) in
a simple theoretical 9ow was computed directly and also
obtained from stretching computations. More than 109 tracer
particles and over 106 stretching values were required to
compute the STD directly and compare it with the prediction
of Eq. (13). Such a level of numerical resolution is usually
impossible and almost always impractical when dealing with
realistic 9ow systems. Eq. (13) cannot be applied directly
to 3D systems such as the example studied here, for several
reasons. First, the value of  is very noisy in 3D systems,
because of limited statistical resolution. Furthermore,  is the
statistical weighting function for H (log s), and it is mainly
determined by the high end tail of H (log ), which is also
very noisy for small data sets.
Fortunately additional theoretical developments allow one
to circumvent the need for direct computation, simply by
recognizing that the high  region of H (log ) has the func-
tional form:

H (log ) ≈ (log  )−1 H (ŵ)e(w−ŵ) =c ; (14)
where ŵ is the mode of w, and H (ŵ) is the value of H (w)
at the mode. The constants C and  can be easily deter-
mined from a linear ;t of a double-logarithmic plot of
the H (log ) data shown earlier in Fig. 10. As shown in
Fig. 11(a) for Re = 50 and in Fig. 11(b) for Re = 100
Eq. (14) accurately captures the high-stretching tail of
H (log ) for several decades of probability. Interestingly,
the ;t improves for larger values of n as the number of
impeller revolutions increases; more and more of the dis-
tribution tail converges toward the expected theoretical
behavior. Somewhat surprisingly, the ;t is better for the
higher value of Re, suggesting that, as intuitively expected,
the strength of correlations for high stretching values is
weaker at higher Reynolds numbers.
Subsequently, H (log s) can be predicted by inserting
Eq. (14) into Eq. (13), i.e., using the ;t, rather than the
original data. H (log s) vs. (−log s) calculated by assuming
so ≈ 1 (the size of the unmixed region initially is assumed
to be of the same order of magnitude as the entire system)
is shown by the dashed curves in Fig. 11(a) for Re = 50 and
in Fig. 11(b) for Re = 100, n = 20 and 60. Since  acts as
a statistical weight on H (log ), H (log s) shifts to the right
of H (log ). In other words, the right branch of H (log )
generates essentially the entire distribution H (log s), and
the mode of H (log s) corresponds to stretching values far
along the high stretching tail of H (log ). This essentially
means that from the narrow viewpoint of generating inter-
material surface for transport, the entire left branch of the
stretching distribution is completely irrelevant.
This observation has deep physical meaning. Fig. 11
corresponding to most of the interfacial contact area in the
stretching events.
3804 E.S. Szalai et al. / Chemical Engineering Science 59 (2004) 3793 – 3805

0 1.0 0
n
-2

log(H(log(s))
-4
-6
-2
-8
10-2
log(H(log(λ))), log(H(log(s)))

-10
-12
-4 -10 10 30 50 70

log(H(w))
-log(s)

-6 10-4

-8
10-6
-10

-12 10-8
-10 10 30 50 70 -8 -6 -4 -2 0 2 4 6 8 10 12
(a) log(λ), -log(s) (a) log(w)

0 1.0 0
-2 n

log(H(log(s))
-1 -4
-6
-2 10-2 -8
-10
log(H(log(λ))), log(H(log(s)))

-3 log(H(w)) -12
-10 10 30 50
-log(s)
-4
10-4
-5

-6
10-6
-7

-8

-9 10-8
-10 0 10 20 30 40 50 60 -8 -6 -4 -2 0 2 4 6 8 10 12
(b) log(λ), -log(s) (b) log(w)

n=20, H(log λ), computed Fig. 12. Main panel: The scaled striation thickness distributions are in-
n=20, H(log λ), predicted variant after 20 periods for both (a) Re = 50 and (b) Re = 100, indicating
n=20, H(log s), predicted that micromixing intensity is independent of agitation rate at low stirring
n=60, H(log λ), computed rates. Inset: log(H (log s)) for n = 20, 40, 60, 80, 100 and 120.
n=60, H(log λ), predicted
n=60, H(log s), predicted

Fig. 11. log(H (log )) for n = 20 ( ) and 60 ( ). The right branch
for n = 20 (—) and 60 ( ) is captured by Eq. (14). log(H (log(s)))
predicted from Eq. (13) for n = 20 (....) and 60 ( ).
The evolution of H (log s), and its scaling properties are
illustrated in Fig. 12(a) for Re = 50 and in Fig. 12(b) for
Re = 100, n = 20–120. The inset shows H (log s) in each
;gure and the main panel shows the same data after the
distributions have been re-scaled by standardization. As re-
vealed in Fig. 12(a) for Re = 50, the shape of the distribu-
tion rapidly approaches a self-similar distribution, where the
curves increasingly overlap one another as n increases. Ac-
cording to Fig. 12(b) the convergence to a self-similar STD
is also fast for Re=100, where the distributions overlap over
three decades of probability for n ¿ 20, and become indis-
tinguishable for over more than ;ve decades of magnitude.
4. Conclusions
The objective of this paper was to analyze 9ow and mixing
in a vessel equipped with Ekato Intermig impellers. We
examined the 9ow ;eld and mixing structures for two cases
in the laminar regime. We showed that despite the complex
9ow ;eld created by the impellers, homogeneous mixing is
not achieved even after several hours of processing time if
highly viscous materials are used.
The computational results for the 9ow ;eld were vali-
dated by comparisons to experimentally measured values.
A laboratory-scale prototype of the industrial mixing vessel
was constructed from clear acrylic and the velocity ;eld at
Re = 37 was measured by Particle Imaging Velocitmetry.
Very good agreement was obtained between the experimen-
tal and simulated 9ow ;elds.
Once the computational tools are validated by experi-
ments, they can be used to evaluate mixing performance and
predict macro- and micromixing eBciency. In this paper we
 E.S. Szalai et al. / Chemical Engineering Science 59 (2004) 3793 – 3805
applied computational techniques to examine the evolution
of mixing patterns and predict severe vertical segregation
at low agitation rates. It was shown that a separation plane
exists in the tank at mid-height from top to bottom, and this
plane forms a signi;cant barrier to mixing in the axial direc-
tion. Convective mixing is very slow at constant agitation
rate across the mid-plane.
It was also shown that slow-mixing regions form around
recirculating loops in the 9uid at low agitation rates. The
shape, size and location of these islands is non-intuitive,
but can be accurately predicted by the computational mix-
ing patterns. The mixing structure at each impeller speed
evolves along a self-similar template that is controlled by
an invariant ;eld of orientations.
Understanding this property of laminar chaotic 9ows of-
fers a solution to the axial segregation problem. Varying the
agitation rate at periodic intervals of time breaks the vertical
separation plane, because the mixing pattern changes at each
di@erent agitation rate. Using the variable rpm technique,
convective mixing occurs in the axial direction signi;cantly
faster than at a constant rate of agitation.
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