Professional Documents
Culture Documents
Roland Lipp
H. Berstorff Maschinenbau GmbH, Hannover, Germany
Evan Mitsoulist
Department of Chemical Engineering, University of Ottawa, Ottawa, Ontario, KIN 9B4, Canada
Numerical simulations have been carried out using the finite DRYING
element method (FEM) for the forming flow of ceramic f CHANNEL I
UNIT 1
tapes. The flow domain encompasses both the slurry reser-
voir and the doctor-blade region with free surface and is
fully two-dimensional. The material of this study is an TAPE
organic-bonded alumina slurry used in a previous experi-
mental investigation and is modeled as a viscoplastic Bing- VB SUPPORT BELT
ham fluid with a yield stress. For different substrate speeds, (a) Doctor-blade casting
the entire flow domain is analyzed and the extent and shape
of yielded/unyielded regions are found. The computed free
FORMING LIQUID CERAMIC
surface profiles are in close agreement with the experimen- TAPE
tal ones. Large vortices appear in the reservoir and their
intensity is computed under different operating conditions.
The lubrication approximation theory (LAT) is then used to
deduce a new reservoir design with tapered walls avoiding TABLE
recirculation. Subsequent FEM studies show the adequacy
(b) Batch casting
of the new design to achieve certain criteria such as elimina-
tion of vortices and an evenly distributed unyielded region.
It is proposed that a combination of LAT and FEM tech- DRYING ZONE
I. Introduction
The forming process of ceramic layers is an essential step which FLOAT GLASS SHEET
influences the properties of the semifinished articles (especially
the dried ceramic sheets) as well as the final products. (c) Rotation casting
The production of ceramic sheets can be carried out as shown
in Fig. 1 with one of the following processes: (a) doctor-blade Fig. 1. Schematic diagram of different tape casting machines: (a)
casting, (b) batch casting, (c) rotation casting. The last is a doctor-blade casting, (b) batch casting, (c) rotation casting.
newly developed process' for continuous production on a solid
glass sheet and is especially suited for making thin multilayer
tapes. Each process comprises (I) the forming of a liquid removal as a dry sheet, as shown schematically in Fig. 1. Usu-
ceramic sheet by using refined ceramic slurry on a support belt ally the forming units are based on the blade-coating principle'
or a glass sheet, (11) the drying of the wet sheet, and (111) its (see Fig. 2 ) .
Detailed information of the forming process is especially of
interest for the production of grain-oriented ceramic^^,^ and for
slurries with tendencies to build textures.' In both cases the par-
G. L. Messing-contributing editor ticle orientation degree should be the same all over the ceramic
tape either to achieve certain properties (e.g., high density) or
to avoid failures (e.g., tension tears). Particle alignment in the
Manuscript No. 195714. Received May 7, 1992; approved October 29, 1992. green sheet is caused by the forming process as shown by Wata-
Supported by the scientific committee of NATO arranged by the Deutsche Aka- nabe et ~ 1 The . degree
~ of particle orientation showed depen-
demische Austauschdienst (DAAD) and by the Natural Sciences and Engineering
Retsearch Council of Canada (NSERC). dence on the shear rate (main flow parameter influencing the
Author to whom correspondence should be addrersed. orientation) under a certain value of the shear rate. Seidemann'
2.54
January 1994 Numericat Flow Simulation of Viscoplastic Slurries and Design Criteriafor a Tape Casting Unit 255
described the correlation between the shear rate distribution of a Experiments were conducted on a tape casting machine (see
viscoplastic slurry and the degree of orientation, which shows Fig. l(a)). The forming unit uses a blade casting tool (Fig. 2).
no particle orientation inside the plug region and increasing ori- The channel gap H was 1.5 mm and the channel width in the
entation degree with increasing shear rate. Consequently, third dimension was 200 mm. A support belt was used having a
regions of small shear rates, such as, for example, plug regions width of 240 mm. Its speed was kept constant at V , = 7.58
in viscoplastic flow, have to be avoided to reach an equal degree mm/s by electronic control.
of particle orientation. The slurry used was an organic-bonded alumina slurry. It
Mathematical modeling and numerical simulations are the consists of a-Al,O, powder, cellulose acetate (binder), dibutyl
favored investigation methods because of the small size of the phthalate (plasticizer), fish oil, acetone (solvent), and cyclo-
hexanone (solvent). The density of the slurry was measured at
area of interest, which makes it very hard for detailed measure-
ments. Usually, the support belt speed and liquid thickness can p = 1825.5 * 0.7 kg/m7.
be measured for a certain design. Numerical simulation can The slurry rheology was determined with a Couette rheome-
provide other critical details, such as regions of recirculation, ter (Rheotest 111) employing a system of coaxial cylinders. The
yieldedhnyielded regions in cases of viscoplastic materials, measured data were assumed to obey the Bingham model
and stresses in the flow field.
Previous theoretical analyse~'.~'have used only one-dimen-
7 = Tv + pj (1)
sional models and simple rheological equations (Newtonian, with a yield stress (found by extrapolation) T~ = 12.1 Pa and a
Bingham, or power-law fluids) to describe and design the blade viscosity p = 4.46 Pa-s in the range of shear rates 0 < j <
channel. However, the complete flow field including the reser- 10 s-'.
voir and the meniscus at exit is hardly one-dimensional, and Surface tension measurements on a ring tensiometer gave a
rheological data for the slurries used are seldom fitted by such value for the surface tension of the slurry u = (29.31 ?
simple equations. 0.15) x 1 0 - 3 ~ 1 ~ .
The assumption of ceramic slurries behaving as viscoplastic All measurements and experiments were undertaken at 20°C
fluids is of particular interest, because such behavior can be room temperature. More details about the experiments, the
approximated by the Bingham model with a yield stress T~and a refinement process, and further data about the slurry (e.g., par-
plastic viscosity p. This model assumes that a fluid behaves as ticle analysis) are given elsewhere. I 4
a solid body at stresses below 7,.
In recent years, a renewed interest has surfaced for the flow 111. Mathematical Modeling of the Forming Process
analysis of viscoplastic materials. Following a seminal paper by
Bird et al. ,* who give a thorough review of viscoplastic materi-
(1) Conservation and Constitutive Equations
als up to the early 1980s, a series of investigations appeared to
study viscoplastic flow, usually with the Bingham model (see The analysis of ceramic tape casting will be carried out under
recent review by Abdali et ~ 1 . ~A) novel
. constitutive equation the assumptions of steady-state, two-dimensional, laminar, and
has been proposed by Papanastasiou," equally valid in both isothermal flow with free boundaries. The conservation equa-
yielded and unyielded regions, thus making it easier to track tions of mass and momentum for an incompressible fluid are
down such surfaces. Such a model has also been used by Abdali 0.8 = 0 (2)
~ the entry and exit flows of Bingham plastics in
et ~ 1 to .study
planar and axisymmetric contractions. pvvv = -vp + v - 7 + pg (3)
Whether or not a true yield stress exists at low shear rates has
where B is the velocity vector, p is the pressure, 5 is the extra
been the subject of intense debate in the scientific commu-
nity. ''-I3 Earlier investigations of alumina slurries showed that stress tensor, p is the density, and g is the acceleration due to
no yield stress could be found.5 These slumes exhibited a sud- gravity.
den increase in the viscosity at low shear rates (below 1 s-'), The constitutive equation that relates 5 to the velocity gradi-
ents VV is a modified Bingham viscoplastic equation proposed
which might be interpreted as corresponding to a yield stress.
Also the difficulty of making such measurements in the low by Papanastasiou'" incorporating an exponential term to control
shear region adds another complication. Special equipment is the stress growth before yielding and is written as
needed'' and avoidance of large errors in the data is not guaran-
teed. Usually reliable data are available only at higher shear (4)
rates, and yield stresses are assumed and extrapolated. This
seems to be a reasonable engineering approximation, and the where p is a constant viscosity, T~ is the yield stress, and rn is
assumption of no deformation under a certain yield stress value the stress growth exponent. The magnitude 191 of the rate-of-
in rheological equations leads to acceptable results for the
description of viscoplastic materials such as ceramic slurries.
+
strain tensor 7 = Vti VvT is given by
The assumption of viscoplastic behavior with a yield stress
for ceramic slurries can thus be viewed as a worst-case sce-
nario, taking into account that the presence of yield surfaces
256 Journal of the American Ceramic Society-Loest et al. Vol. 77, No. 1
where 11, is the second invariant of the extra stress tensor. Note
that previous work by Papanastasioul"and Beverly and Tanner" For the viscoplastic materials used in this work, St =
employed thccriterion of the second invariant of the rate-of- O(O.1-1), and the gravity term has to be included in the
strain tensor exceeding an arbitrarily small value -jc close to equations.
zero. As argued by Abdali et a1.,9 such a choice may lead to The relative importance of pressure forces compared to vis-
noncomparable and/or ambivalent results. On the other hand, cous forces in the equation of momentum is assessed by the
using as a criterion the value of yield stress, which is not arbi- Hagen number, defined by
trary but a given constant, reduces the uncertainty of using val-
ues very close to zero, which may be numerical noise.
(2) Dimensionless Groups
Ha = -
\ I
I-
-\=\g y=o
Fig. 4. Schematic diagram ofthe tape casting equipment along with notation and boundary conditions for flow analysis.
for the mass and momentum equations using the primitive vari- x (mm)
able approach, i.e., velocities and pressure (u-v-p formula- 1.8
tion). Streamlines are obtained a posteriori by solving the 1.2
Poisson equation. More details about the solution process can 0.B
0.4
be found in Ref. 17.
0.0
104.0 105.0 106.0 107.0 108.0 109.0 110.0 111.0 112.0 113.0
Fig. 5. Finite element grids used (a) in the entry section and (b) in
(2) VerticalReservoir the exit section of the tape casting domain.
The numerical simulations have been initially carried out in
the experimental design apparatus of Fig. 2, comprising the
slurry reservoir with vertical walls, the channel and the exit Table I. Viscoplastic SimulationResults for Slurry Used in the
region in an effort to compare the results with the experimental Experiments
findings. The domain exit has been set at 6 mm from the chan- Case. V,(mm/s)' h(mm)* Bi' Re' st" Cat*
nel exit (or 4H), which was found sufficient to achieve a flat I 3.79 0.819 0.59 1.3 X lo-' 0.71 0.58
velocity profile with no further changes occurring. I1 7.58 0.786 0.28 2.5 x lo-' 0.32 1.15
The calculations have been performed with several grids to I11 15.16 0.769 0.14 4.8 X 0.14 2.31
establish results independent of mesh influence. Typical grids 'Belt speed. 'Coating thickness. 'Bingham number. 'Reynolds number. "Stokes num-
in the entry and exit regions are shown in Fig. 5. They contain ber. **Capillarynumber.
258 Journal of the American Ceramic Society-Loest et al. Vol.77,No. 1
where JIB and $c are the stream function values at the support 16.0
belt and coating surface, respectively. Thus, a value of 1 corre-
sponds to the flow rate and negative values correspond to a per-
centage of the fluid recirculating in the opposite direction from v
E 12.0
20 0
els. The unyielded regions tend to form near the reservoir top, h
near the right wall, and the upper half of the vortex. At the 80
highest speed of 15.16 m d s , they have virtually disappeared in
the vortex region. The corresponding yielded/unyielded
regions after the exit are shown in Fig. 7 along with the stream- 40
gravity and viscous forces has been used up. Shorter channels
would produce coatings determined not solely by the dragging 0.0
action of the belt but by the pressure forces as well. The final -20.0 -15.0 -10.0 -5.0 00 50 LO 0
pressure value on the belt after the exit corresponds to pgh due x (mm)
to gravity.
The shear stress distributions along the belt are shown in Fig. Fig. 6 . Streamline patterns in entry flow of ceramic slurry from the
9 for the three different belt speeds. Again negative high peaks reservoir into the blade channel for different belt speeds (unyielded
appear at the impact region (point A) and then there is a pro- regions are shaded). Data given in Table I.
gressive buildup of stresses before entrance to the blade channel
(point E) where a leveling-off occurs due to the straight channel
geometry. At exit from the blade channel (point D), the shear for the surface tension terms in the finite element program.
stresses quickly drop to zero. It is seen that everywhere on the Quadratic interpolation would certainly improve the curvature
belt the absolute shear stress values exceed the yield stress as x 4 0. The other two cases gave similar shapes both experi-
(7, = 0.0121 kPa), except in the free surface region. mentally and numerically and are not repeated here.
A typical comparison between the experimentally found free
surface shape and the numerical simulations for VB = 7.58 (2) Tapered Reservoir
mm/s (case 11) is shown in Fig. 10. A good agreement is It is well known that tapered reservoirs are sometimes used in
obtained, especially for the final coating thickness (error tape casting to improve the product quality. It is argued here
<I%), but the numerical results tend to underestimate the that such geometries are necessary to eliminate the vortices and
experimental free surface curvature. The discrepancy we produce a smooth streamlined flow pattern. Fluid recirculating
believe is mainly due to the use of linear interpolation functions in large areas may eventually come out of the machine having
January 1994 Numerical Flow Simulation of Viscoplastic Slurries and Design Criteriafor a Tape Casting Unit 259
Fig. 8. Pressure drops along the support belt for different belt speeds Note also the dependence of Ha on the flow rate Q:
in tape casting of ceramic slurry.
Fig. 11. Finite element grid used in the modified design A with a
Fig. 9. Shear stress distributions along the support belt for different tapered reservoir wall to eliminate recirculation according to the lubri-
belt speeds in tape casting of ceramic slurry. cation approximation theory (LAT).
260 Journal of the American Ceramic Society-Loest et al. Vol. 77, No. 1
24.0 , * I ,
24 0 I I I
1.0
0.0 J
7
E 120
h
E
E I20
v v
>> x
80 8.0
40 4.0
00 00
-300 -250 -200 -150 -100 -50 0.0 5.0 100 -21.0-18.0 -15.0 -12.0 -9.0 -6.0 -3.0 0.0 3.0 6.0 9.0
0.1 24.0 I
24 0
P;O
20 0 20.0
DESIGN B
1G 0 16.0 Case I1
E E
120
1
12.0
v v
x x
80 8.0
40 4.0
00 0.0
-300 -250 -200 -150 -100 -5.0 0.0 5.0 10 0 -210-180 -150 -12.0 -9.0 -8.0 -3.0 0.0 3.0 0.0 9.0
1.0 r
24.0
20 0
16 0 Lh IG 0
v
E I20
80
40
to give Ha < 2 . This is necessary when H , p, and V , are fixed. same number of elements and nodes have been used as before to
The present length of L = 107 mm is long enough to always ensure results free from mesh influence.
give Ha < 2. The streamline patterns together with yieldedlunyielded
Knowing the rheological constants and support belt speed, it regions for different speeds are shown in Fig. 12. The vortices
is possible to solve for the maximum height H of the channel, have been successfully suppressed, and a smooth streamline
by requiring that the shear rate become zero on the blade wall. pattern exists for all belt speeds. The unyielded regions are
This guarantees that no negative velocities are obtained any- more evenly distributed in the reservoir and are reduced in size
where in the channel, thus avoiding recirculation. This method as the belt speed increases. At the highest speed, the unyielded
applied to the present data and for V , = 7.58 m d s gives regions are limited to the top and near the left reservoir wall.
H , , , = 2.3 mm. The corresponding pressure drop along the lower tapered
We have therefore modified the design of Fig. 5 to add a reservior wall and support belt is shown in Fig. 13 for case I1
tapered section in the reservoir running parallel to a tapered (belt speed V , = 7.58 rnds). Again high peaks appear at
section of the blade going from H to H,,,. Thus, we do not impact point with the belt (point I). The channel is long enough
allow the fluid to flow under drag in a channel having a height to have used up all pressure drop in it, so that the coating thick-
greater than H,,,. We have kept about the same reservoir length ness is mainly determined by the dragging action of the belt.
and the same height. The new design (called design A) and its A further design modification is possible to eliminate the
finite element discretization are shown in Fig. 1 1 . About the large unyielded regions on the left reservoir wall as well as the
January 1994 Numerical Flow Simulation of Viscoplastic Slurries and Design Criteriafor a Tape Casting Unit 26 1
0.5
I
=o
n
0.4
v,(l)
Is
$
4: 0.3
W
Ck
6 0.2 H
k
2
g 0.1
k
a
0.0
__t
VX(0) 1
-0.1 I1 I I
-30.0 0.0 30.0 60.0 90.0 120.0 Fig. A l . Fully developed combined pressure and drag flow of a Bing-
x (mm) ham plastic in a straight channel.
Fig. 13. Pressure drop along the lower tapered reservoir wall and
support belt for belt speed V, = 7.58 mm/s (case 11, design A).
(A-2~)
(A-2b)
dead region near the tapered blade channel after entrance. We
refer to the new modified design as design B. The corre-
sponding streamline patterns with yieldedhnyielded regions and the boundary conditions are
are also shown for comparison in Fig. 12 for the three different (BCI) v,(y) = V, (aty = 0) (A-3a)
belt speeds. It is evident that design B satisfies the criteria set
forth above, i.e., elimination of recirculation and reduction of (BC2) v,(y) = 0 (aty = H ) (A-36)
the unyielded regions. The pressure drops and shear stress dis- By setting dimensionless variables
tributions show similar trends as in the previous designs and
will not be repeated here.
V. Conclusions
The flow of ceramic slurries inside tape casting equipment
has been analyzed using the finite element method. Rheological
data for an organic-bonded alumina slurry [a-A1,OT powder, (A-5)
cellulose acetate (binder), dibutyl phthalate (plasticizer), fish and dropping thereafter the asterisks we obtain upon integration
oil, acetone (solvent), and cyclohexanone (solvent)] have been of Eq. (A-1)
fitted with a viscoplastic Bingham model incorporating a stress
growth exponent which makes it valid in both yielded and 7 HWYo - Y)
= ('4-6)
unyielded regions. The full 2-D analysis gives a good
agreement between the computed free surface profiles and the where yo is the position of zero shear stress.
experimental observations. The extent and shape of yielded/ From Eqs. (A-2a) and (A-6) we obtain
unyielded regions is also found for different support belt 1 dv
speeds. The computations show that reservoirs with vertical + --
Bi dy
= HB(yo - y) (A-7)
walls and an open side to the moving belt have always large vor-
tices in the absence of externally imposed pressure forces (drag- and the location of the plug region ypwhen dvldy = 0, i.e.
dominated flow caused by the belt). Elimination of these vorti-
ces is possible by modifications in the reservoir and blade ypl = yo - I/HB (A&)
design, incorporating tapered walls to produce smooth stream-
line patterns. The use of the lubrication approximation theory
yp2 = yo + 1/HB (A-8b)
(LAT) is useful for easily determining design changes to meet For the solution of Eq. (A-7) we can distinguish the following
certain criteria. As such we set forth here mainly the absence of three cases:
recirculation in the reservoir and the reduction of unyielded
regions in order to produce ceramic tapes free of defects caused Case A-no plug, Ha < 2
by the rheological flow behavior of the slurries. 1-Bi
Y o = T + -21 64-91
APPENDIX
The lubrication approximation theory (LAT) gives for the (A-10)
case of a fully developed combined pressure and drag flow of a
viscoplastic Bingham fluid in a straight channel' (see also Fig. Case B-plug on the wall, 2 < Ha < Ha,-, where
'41)
Ha,_, = 2Bi +1+ ,/4= (A-1 1 )
where - -1-'
0 - HB -& (A- 12)
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I
- Ha
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