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Chemical Engineering Science 65 (2010) 5699–5715

Contents lists available at ScienceDirect

Chemical Engineering Science


journal homepage: www.elsevier.com/locate/ces

Local analysis of the tablet coating process: Impact of operation conditions


on film quality
Daniele Suzzi a, Stefan Radl a,b, Johannes G. Khinast a,b,n
a
Research Center Pharmaceutical Engineering GmbH, Graz, Austria
b
Institute for Process and Particle Engineering, Graz University of Technology, Inffeldgasse 21a, Graz, Austria

a r t i c l e in fo abstract

Article history: Spray coating is frequently used in the pharmaceutical industry to control the release of the active
Received 3 August 2009 pharmaceutical ingredient of a tablet or to mask its taste. The uniformity of the coating is of significant
Received in revised form importance, as the coating usually has critical functional properties. However, coating uniformity is
15 July 2010
difficult to predict without significant experimental work, and even advanced particle simulations need
Accepted 16 July 2010
to be augmented by CFD models to fully describe the coating uniformity on a single tablet.
Available online 6 August 2010
In this study we analyze the coating process by using detailed computational fluid dynamics (CFD)
Keywords: multiphase spray simulations. The impact and the deposition of droplets on tablets with different
Multiphase flow shape, as well as the production and evolution of the liquid film on the surface of the tablets are
Simulation
numerically modeled. Spray droplets are simulated with a Discrete Droplets Method (DDM) Euler–
Mass transfer
Lagrange approach. Models for multi-component evaporation and particle/wall interaction are taken
Pharmaceuticals
Tablet coating into account. The wall film is treated with a two-dimensional model incorporating submodels for
Spray interfacial shear force, film evaporation and heat transfer between film, solid wall and gas phase. Our
simulations show how different physical parameters of the coating spray affect the coating process on a
single tablet. For example, we analyze for the first time the deposition behavior of the droplets on the
tablet. The outcome of our work provides a deeper understanding of the local interaction between the
spray and the tablet bed, allowing a step forward in the design, scale-up, optimization and operation of
industrial coating devices. Furthermore, it may serve as a basis for the combination with state-of-the-
art DEM particle simulation tools.
& 2010 Elsevier Ltd. All rights reserved.

1. Introduction the film thickness varies between 5 and 100 mm. A detailed
description of the coating process and the different coater devices
Coating is an important step in the production of many solid is presented in the book of Cole et al. (1995).
oral dosage forms, such as tablets and granules. The goal of film Historically, this process was developed by the confectionery
coating is the application of a thin polymer-based film on top industry to sugar-coat different types of candies. The
of a tablet or a granule containing the active pharmaceutical pharmaceutical industry implemented this technique using open
ingredients (APIs). In the last years, more than half of all the bowl-shaped pan. Nowadays, sugar-coated tablets are rarely
pharmaceutical tablets were coated (IMS Midas Database, 2007). developed due to the intricacy of the process and the high degree
Functional coatings are usually adopted for taste masking or to of operator skill required. Instead, tablets are typically coated
alter the tablet’s dissolution behavior, for example by controlling with a polymer film of various compositions using modern
the rate of dissolution via semi-permeable membranes or by equipment, such as drum and pan coaters.
making it resistant to gastric juice through enteric coatings. The first commercially available pharmaceutical film-coated
Furthermore, active ingredients may be incorporated in the film tablet was introduced to the market in 1954 by Abbott
layer. Colored non-functional coatings are commonly used to Laboratories. Tablets were produced in a fluidized bed coating
improve visual attractiveness, handling and brand recognition. column based on the Wurster principle (Wurster, 1953), which
A well-known example is the ‘‘blue pill’’ VIAGRAs by Pfizer Inc. was further developed by Merck in their US and UK plants. This
Depending on the tablet’s dimension and coating functionality, new technique could be realized due to the development of new
coating materials based on cellulose derivatives, e.g., hydroxy-
propyl methylcellulose. Nevertheless, in the following decades
n
Corresponding author at: Research Center Pharmaceutical Engineering GmbH,
coating columns were substituted by side-vented pans and the
Graz, Austria. Tel.: + 43 316 873 7978; fax: + 43 316 873 7963. use of aqueous film solutions, which reduce the use of organic
E-mail address: Khinast@TUGraz.at (J.G. Khinast). solvents and the related costs of the recovery systems.

0009-2509/$ - see front matter & 2010 Elsevier Ltd. All rights reserved.
doi:10.1016/j.ces.2010.07.007
5700 D. Suzzi et al. / Chemical Engineering Science 65 (2010) 5699–5715

Nowadays, tablet coating is typically carried out in pan coaters


or fluidized bed systems. Modern production-scale pan coaters
have batch sizes ranging from 500 g to 2000 kg, have a fully
perforated cylindrical drum and use two-material nozzles for an
effective spray generation. Today’s fluidized bed coaters allow
continuous coating or have special internals to allow for coating
processes involving coating solutions with high solid content
(Porter, 2006). In this study we focus on pan coaters.
Although coating processes have been used for many decades,
there are still serious challenges, as there is a lack of under-
standing of how material and operating parameters impact
product quality and cause problems, such as chipping (i.e., films
become chipped due to attrition), blistering (i.e., local formation
of blisters due to entrapment of gas), cratering (i.e., penetration of
the coating solution into the bulk of the tablet causing crater-like
structures), pitting (i.e., pits occur on the surface due to Fig. 1. Schematic of a modern pan coater (side-vented) and domain for the spray
overheating of the tablet and partial melting), picking (i.e., parts analysis.
of the film are removed due to sticking to other wet tablets),
blushing (i.e., formation of spots due to phase-transitions of the
polymer film), blooming (i.e., plasticizer concentrates at the
surface, leading to a change of appearance), film cracking (i.e.,
cracking of the film upon cooling due to high stresses) and many
others. Quite often, poor scale-up of the process and/or insuffi-
cient process understanding is the cause of such production
problems and batch failures Pandey et al. (2006a). Although the
reasons for these manufacturing problems are more or less
understood, it is still a challenge to predict the occurrence of such
effects for new systems.
Therefore, in our work we focus on a basic understanding of
the film formation process on single tablets, with the goal of being
able to predict the impact of material and operation parameters
on the film quality. The current study is a first step in this
direction. We investigate the spray fluid dynamics and the film Fig. 2. Conceptual scheme of the coating process.
formation of a glycerin–water mixture on two different tablet
shapes, i.e., a sphere and a biconvex tablet, held in one position.
Our analysis is based on a rigorous computational model that uses tube system) or through a perforated rotary pan. The latter design
well established physical submodels for momentum, heat and allows the drying air to flow through the tablet bed in co-flow
mass transfer. Thus, we are able to predict the transient with the injected spray, leading to a more efficient coating
development of the mean film thickness of a wetting coating process. Several companies offer this type of equipment, such as
solution on arbitrarily shaped surfaces. Our main objective is to Glatt, Bohle, Driam, Manesty or Nicomac, each system being
provide, for the first time, a science-based and quantitative significantly different to the other systems.
understanding of which physicochemical parameters influence As shown in Fig. 2, the coating process can be divided into three
the uniformity of the coating layer on a single tablet. This phases, i.e., spraying, wetting and drying. In an ideal process, each
knowledge is the key for the design, optimization and the rational tablet or granule passes through the spray zone for a predefined
scale-up of such processes and can form the basis for further number of times, where spray particles impact the surface and wet
studies on rotating tablets or whole tablet beds. the tablet. The adhering film is dried before the next amount of
solution is applied. This process continues until the particle is fully
coated. The final film structure is typically non-homogeneous due to
2. Background the presence of insoluble ingredients, such as pigments, and to the
discontinuous and statistical nature of the coating process. A typical
2.1. Spray system scanning electron microscope (SEM) image of a film-tablet coating
illustrating the inhomogeneity of the coated layer is also shown
A modern coating system is conceptually shown in Fig. 1, in Fig. 2.
where the coating suspension is sprayed on top of a moving bed of Depending on the desired functionality of the tablet film,
the solid dosage form. The spray guns are usually mounted on an different coating solutions are used in industrial practice. The
arm inside the pan and are directed towards the tablet bed. As the injected spray commonly consists of a carrier solution or vehicle
bed is moving, a tablet spends a fraction of a second in the (e.g., water, alcohols, ketones, esters or chlorinated hydrocar-
spraying zone. The wet surface of the tablet needs to be dried to bons), polymers (e.g., cellulose ethers, acrylic polymers or
avoid sticking of the tablet to neighboring tablets, leading to copolymers), plasticizer (polyols as glycerol, organic esters or
manufacturing problems such as picking. However, too fast drying oils/glycerides) and insoluble solid components (e.g., talcum,
is counter-productive as well, as other problems may occur, such pigments and opacifiers). The used vehicle has to be compatible
as the formation of a heterogeneous film. The drying air is with the chosen polymer, as this is essential for obtaining optimal
directed towards the surface of the tablet bed in order to achieve film properties such as mechanical strength and adhesion. As
good heat and mass transfer (i.e., for immediate drying of pointed out by Hogan (1982), the originally used organic vehicles
the sprayed solution). The exhaust air can exit the pan through have been steadily replaced by, mainly due to environmental and
side opening, from inside the tablet bed (through an immersion safety concerns. Several authors (e.g., Bindschaedler et al., 1983)
D. Suzzi et al. / Chemical Engineering Science 65 (2010) 5699–5715 5701

analyzed the complex process of film formation from a water- sulfate instead of dextran. Eliassi et al. (1999) focused instead on
polymer dispersion. Initially, the polymer is dispersed in the the activity of water in aqueous PEG solutions with different
aqueous solution in the form of discrete particles. The dispersed molecular weights. Recent experimental work on PEG solutions
particles have to come into contact, coalescence and finally form a has been extended by Kazemi et al. (2007). The activity of water in
continuous film. aqueous sugar solutions has been analyzed in two studies of Peres
An important factor in the film coating process is the quality of and Macedo (1996, 1997).
the spray, as the droplets interaction with the tablet surface Finally, the interaction between droplets and surfaces
strongly affects the drying behavior and the uniformity of the final represents a key issue in the description of coating processes.
polymer layer. Two types of spraying devices are commonly used Experimental analyses and dimensional modeling of drop splash-
in the film-coating technology: the hydraulic (airless) atomizer ing processes can be found already at the beginning of the 20th
and the pneumatic (air-blast) atomizer. The first device requires century in the work of Worthington (1908). The recent review of
high load pressures in order to produce adequate atomization of Yarin (2006) comprehensively explains the processes leading to
the viscous solutions. However, the absence of air to produce the film formation on thin liquid layers and dry surfaces, i.e., crown
spray reduces early droplet evaporation. In case of aqueous formation or splashing, drop spreading and deposition, receding
vehicles this can lead to product overwetting and to poor-quality (recoil), jetting, fingering and rebound.
coatings. For this reason pneumatic atomizers are mostly used for
water-based coating solutions (Muller and Kleinebudde, 2006). 2.2. Tablet flow in coaters
The liquid jet instability and the atomization processes in these
atomizers have been discussed by several researchers, e.g., Varga
Experimental and numerical studies of the tablet flow in pan
and Lasheras (2003), as well as Mansour and Chigier (1995).
coaters are gaining increasing interest in the scientific commu-
A combined experimental and theoretical analysis of the atomiza-
nity. Sandadi et al. (2004) characterized the movement of tablets
tion of highly viscous non-Newtonian liquids can be found in the
at the top of a granular bed in a rotating pan via a digital imaging
work of Aliseda et al. (2008). In this study the breakup process is
system to measure the velocity distribution on the surface of the
modeled through a two-stage instability mechanism, namely the
tumbling tablet bed. Tobiska and Kleinebudde (2001) investigated
primary Kelvin–Helmoltz instability followed by the secondary
the mixing behavior in a new coater type (the Bohle BLC pan
Rayleigh–Taylor instability. This study starts from the work of
coater). They showed that the mixing behavior can be character-
Joseph et al. (2002), as well as of Yecko and Zaleski (2005). The
ized by a simple temperature measurement, i.e., the temperature
main result of Aliseda et al. (2008) is a correlation between the
difference between the spray and the drying zone. In another
Sauter mean diameter (SMD) of the disintegrating droplets and
study the same authors characterized the coating uniformity in a
the atomizer geometry, as well as the fluid-dynamical properties
Bohle lab-coater using standard procedures (mass variance,
of the injected liquid (they used a solution of water and glycerol).
dissolution testing) (Tobiska and Kleinebudde, 2003).
In the absence of direct measurements of the real spray, e.g.,
Pandey et al. (2006b) tracked a single tracer tablet (white
through Laser Diffraction (LD) or Phase Doppler Anemometry
colored) in a bed of black tablets using a CCD camera. They
(PDA) systems (Hirleman, 1996), these models may be helpful for
recorded the centroid location, as well as the exposed area of the
the initialization of the ‘‘numerical spray’’. This approach is, for
tracer tablet in the zone of interest, i.e., the spray zone. The
example, also adopted in our work, i.e., our simulations are based
camera was directly placed in the coater and oriented in the same
on a single mean diameter of the droplets that make up the spray.
direction as the spray. They analyzed the average surface velocity
The liquids being atomized are often highly viscous and
profile along the upper layer of the tablet bed. In addition, Pandey
sometimes non-Newtonian fluids, exhibiting complex physical
et al. (2006a) performed discrete element method (DEM) simula-
mechanisms for primary and secondary breakup. In addition,
tions confirming the shape of the velocity profiles along the top
droplet formation is also strongly affected by other physical
cascading layer of the tablet bed. The range of the velocities
properties of the coating solution, e.g., density and surface
reported varied between 0.13 and 0.55 m/s. Pandey et al. (2006a)
tension, as well as by the spray gun type. For example, Aulton
proposed a characteristic velocity V for the purpose of scaling the
et al. (1986) investigated the effects of different atomizers, such as
velocity profile at the top of the granular bed:
Binks-Bullows, Walther Pilot, Schlick and Spraying Systems guns,
 g 1=6
showing strong effects of the atomizing air pressure on the V ¼ kRN 2=3 v1:8 ð1Þ
resulting mean droplet diameter. Typical mass-averaged droplet d
sizes range between 20 and 100 mm. The atomization properties, Here k is a constant, R is the pan radius, N is the pan rotation
such as droplet size and velocity distribution, can be experimen- rate, g is the gravitational acceleration and d is the tablet size. The
tally obtained via captive methods (these are methods in which term n represents the fractional fill volume, defined as the ratio
droplets impinge on a flat surface and the diameter of the droplets between the volume occupied by the bed and the total pan
on the surface is measured using a microscope), photographic volume. The relation was verified using experimental data
techniques or laser-light scattering methods (Lefebvre, 1989). between n ¼0.10 and 0.17 and rotational speeds between o ¼6
Clearly, the characterization of the coating spray represents an and 12 rpm. Alexander et al. (2002) used a similar approach and
important step in the design of a coating device, as it strongly scaled the maximum velocity at the top of the granular bed to
S
affects the local behavior of the film formation on the tablet obtain a dimensionless maximal velocity Vmax . For low rotational
surface. speeds ( o30 rpm), they found that the value of Vmax S
is between
The evaporation of individual species from the liquid phase 2.5 and 3.8. All these scaling laws are useful for the estimation of
making up the droplets has to be considered as well. It is clear the peak velocity in coaters and consequently for the time
that the composition of the droplets affects the mass transfer from individual tablets stay in the spray zone.
the spray droplets and the tablet film to the surrounding gas. For Kalbag et al. (2008) used a single tracer sphere and a digital
example, Chen and Thompson (1970) investigated the effect of camera to measure the time that the marked tablet remains in the
sodium chloride on the vapor–liquid equilibrium of glycerol– spray zone, also called spray residence time tR. They manually
water solutions. Gaube et al. (1993) studied aqueous solutions of post-processed the videos (50 min runtime at 60 fps) to obtain
PEG (often used in coating formulations) and dextran. A similar consistent experimental results for the spray residence time. The
system was also studied by Hammer et al. (1994), using sodium authors defined the dimensionless appearance frequency ai of
5702 D. Suzzi et al. / Chemical Engineering Science 65 (2010) 5699–5715

tablet i as the number of appearances of a tablet in the spray zone consider the deposition of droplets on the tablets, nor the film
during one pan revolution. The dimensionless appearance formation processes. The recent paper by Freireich and Wassgren
frequency averaged over all tablets a can be expressed as (2010) examined both analytically and computationally the
   influence of a tablet’s orientation on the coating uniformity,
2p n
a¼ ð2Þ leading to a deeper understanding of the intra-tablet film
o N
variability.
Here DtR is the average residence time per pass in the spray
zone averaged over all tablets. The averaged dimensionless
appearance frequencies were between a ¼ 0:1 and a ¼ 1:4. 3. Objectives
However, this value depends strongly on the coating fraction,
i.e., the ratio of the average number of tablets exposed to the Currently, the optimization of industrial coaters is mostly done
spray and the total number of tablets in the coater. Therefore, by means of experimental and empirical analysis. State-of-the-art
they proposed an average residence time of the tablets per pass, computational approaches include the use of Discrete Elements
i.e. DtR ¼ L=V. Here L is the length of the spray zone and V is the Method (DEM) , which already represents a consolidated practice
average velocity of tablets passing through the spray zone. The in particle technology. However, current studies lack a detailed
velocity at the top of the tablet bed is essential for the residence description of the film formation process on individual tablets or
time in the spray zone, and hence, is expected to impact the film granules as only statistical tools for the film deposition on the
quality on the tablet. The average residence time of the tablets per tablet surface are used. Such an approach cannot capture the local
pass was found to be between 0.07 and 0.27 s, depending on the behavior of the complex particle–gas–liquid system. Clearly, the
pan speed. The standard deviation of the average residence time liquid deposition behavior is strongly affected by the interactions
per pass was in the order of 0.03–0.24 s and was strongly of the spray and the solid surface of the tablet to be coated. Hence,
dependent on the chosen pan speed. These experimental results the presented work will focus on the understanding of the basic
were reproduced by discrete element method (DEM) simulations. principles of the spraying and deposition processes on a single
Clearly, the standard deviation is an important quality tablet or granule as shown schematically in Fig. 2.
indicator for the coating uniformity as tablets with a short In summary, the major objectives of this work are
residence time in the spray region will have a thin or imperfect
coating. Also, in their work Kalbag et al. introduced other metrics  to model the spray, deposition on the tablet, the coating
that characterize the mixing behavior in the bed, i.e., the process, as well as the evaporation of the spray and the wall
circulation and the fractional residence times. The circulation film in order to estimate the effects of the drying gas flow,
time tC,i and the average circulation time per pass DtC characterize  to numerically analyze the impact and deposition of droplets
the total time the tablet spends away from the spray zone, and the on particles with different shape,
average time interval between successive appearances of the  to study the production and evolution of the liquid film on the
tablet in the spray zone, respectively. Note that the sum of the surface of the tablets and
tR and tCi is the total coating time. The fractional residence time fR  to investigate how different process parameters affect the
is defined as the ratio of time spent by a tablet in the spray zone to coating process on a single tablet.
the total coating time t0. The average fractional residence time is
For this purpose, a variation matrix was set up and the effect of
tR n
fR ¼ ¼ ð3Þ each variation is analyzed in detail with respect to the film
t0 N
quality. Also, the shape of the coated particle is varied, i.e., by
where tR is the average time the tablets spend in the spray zone, considering a sphere and a standard tablet.
n is the average number of tablets in the spray zone and N the
total amount of tablets inside the pan coater. The ratio n=N is also
referred to as the ‘‘coating fraction’’ and can be increased by 4. Model and numerical solution
increasing the size of the spray zone or by decreasing the number
of tablets in the coater. In this section we present the 3D model used for the numerical
Theoretical models for predicting the surface renewal rates of analysis of the spray and the wall film. We adopted the 3D-CFD
the tablet bed in a rotary coating drum were reported by Denis code AVL FIRE v2008 to simulate the dynamics of the coating
et al. (2003). They found an excellent agreement between the spray and the film evolution on the tablet. We treat the coating
prediction of their model and experimental results for spherical process as a gas–liquid multiphase flow with deposition of a
tablets and bifluid pneumatic nozzles. liquid film on the surface. For the description of the gas flow
Different groups are currently working on the numerical around the object to be coated we used the Reynolds averaged
prediction of tablet flow in coaters (e.g., Dubey et al., 2008; Navier–Stokes (RANS) equations including an appropriate turbu-
Pandey et al., 2006a; Yamane et al. 1995). The coating event in the lence model (k–e). As these models are well-known they are not
spray zone has up to now been described only with discrete described here. The main difficulty of our work is to accurately
element methods (DEM) and statistical deposition models for the model the motion of individual droplets, i.e., the spray around the
tablets crossing the droplets region. One of the first attempts to object, as well as the droplet deposition and the motion of the
couple a DEM solver with the computational fluid dynamics (CFD) liquid already deposited on the tablet surface.
gas flow in a rotating drum was proposed by Nakamura et al.
(2006). However, they simply assumed that a tablet was coated if 4.1. Spray simulation
it was located within the spray region. This approach neglected
resolving the droplets motion inside the drum and the local In our work the simulation of sprays is performed via the
interaction of impacting drops on the tablet surface. Few Lagrangian DDM (Discrete Droplet Method) approach. This
additional studies have been reported on the CFD simulation of approach is also known as Lagrangian Monte Carlo method,
coating processes. The recently presented work of Muliadi and which was first proposed by Dukowicz (1980). The basic concept
Sojka (2009) analyzed the interaction between coating spray and is to track the paths of statistical parcels of real droplets
air flow inside a pan coater. However, the authors did neither in physical, velocity, radius and temperature space. Further
D. Suzzi et al. / Chemical Engineering Science 65 (2010) 5699–5715 5703

submodels for drag, particle/wall interaction, evaporation, turbu- mixture of components, i.e., glycerol and water, the calculation of
lent dispersion and breakup may be included in the simulation the mass transfer rate (i.e., the evaporation process) represents a
approach. In the DDM method each physical phenomenon key challenge in the simulation model. The multi-component
occurring in a parcel, e.g., atomization or coalescence/collision, evaporation model used in this work is based on the Abramzon
directly involves all the droplets making up the parcel. This allows and Sirignano (1988) approach with the extension by Brenn et al.
a drastic reduction in the computational effort to simulate liquid (2003). The main difference to the single-component case is that
sprays, which in reality consist of many millions of single drops. mass transfer of every component is taken into account
In our simulations, the effects of secondary atomization, separately, while heat transfer is still globally described. Hence,
collision and coalescence have been neglected. We are aware the evaporation rates of each species j are calculated and summed
that close to the nozzle outlet this assumption is not valid due to up to yield the total mass loss due to evaporation:
the high droplet number density and velocity. For example X
m_ iE ¼ m_ iE,j ð10Þ
Edelbauer et al. (2006) and Suzzi et al. (2007) showed that the j
high liquid volume fraction close to the nozzle compromises the
basic assumptions of the Lagrangian particle method. In this study In the multi-component evaporation model used in this work,
we circumvent these difficulties by initializing the spray just the mass transferred for each component j to the gas phase is
outside the primary breakup region, a few centimeters down- given by
stream the nozzle outlet. We then can neglect secondary breakup _ iE,j ¼ prg bgj Dd Shj lnð1 þ BM,j Þ
m ð11Þ
effects, as the Weber number of the droplets is, in our application,
The overbars in the gas density rg and the binary diffusion
far away from critical values.
coefficient bgj of species j in the gas phase indicate that these
Mass, momentum and energy conservation equations are
values are evaluated at a reference temperature and composition
solved for each parcel i of the spray. A parcel represents a certain
(for more details refer to AVL, 2008). Dd is the droplet diameter,
number of individual droplets, depending on their radius and
Shj is the corrected Sherwood number of species j (defined below)
the spray rate. The continuity equation for each parcel can be
and BMj is the Spalding mass transfer number defined as
written as
wj,s wj,1
dmid BM,j ¼ ð12Þ
_ iE
¼ m ð4Þ 1wj,s
dt
Here, wj,s is the gas phase mass fraction of species j at the
where the term on the right hand side represents the mass source
surface of the drop (to be calculated from the vapor pressure of
due to evaporation. In the Lagrangian DDM the momentum
species j at the droplet temperature) and wj,N is the bulk gas
equation, i.e., Newton’s second law, is directly integrated over
phase mass fraction. The total mass transfer rate can be also
time for each spray parcel:
derived from the energy balance (Eq. (9)) at the surface of the
! drop, as
d u id ! ! ! !
mid ¼ F iD þ F iG þ F iP þ F iEX ð5Þ
dt kg
The terms on the right hand side of Eq. (6) represent the drag _ iE ¼ p
m D Nu lnð1 þBT Þ ð13Þ
cp,d d
force FiD, the gravity and buoyancy force FiG, the pressure force FiP,
and the external force FiEX. The drag force acting on the droplets is Here, kg is the heat conductivity at a reference temperature and
calculated as composition, and Nun is the corrected Nusselt number defined
below. In order to account for the relative motion between spray
! 1 ! !
F iD ¼ rg Ad CD 9 u rel 9 u rel ð6Þ particles and gas phase, a Nusselt and Sherwood number is first
2
computed according to the empirical relations of Ranz and
where rg is the gas density, Ad the cross-sectional area of the Marshall (1952):
!
droplet and u rel the relative velocity between the gas phase and
Nu0 ¼ 2 þ 0:552Re1=2 Pr 1=3 ð14Þ
the parcel. The term Cd represents the drag coefficient for a single
sphere and is modeled in our work according to the formulation of
Sh0,j ¼ 2 þ 0:552Re1=2 Scj 1=3 ð15Þ
Schiller and Naumann (1993):
8 The corrected Nusselt and Sherwood numbers Nun and Shj are
< 24 ð1 þ 0:15Red 0:687 Þ, Red o103
>
then calculated taking into account the deviation of the
CD ¼ Red ð7Þ streamlines due to the evaporating mass flow:
>
: 0:44, Red Z103
ðNu0 2Þ ðSh0,j 2Þ
Here the particle Reynolds number Red is defined as Nu ¼ 2 þ , Shj ¼ 2 þ ð16Þ
FT FM,j
rg 9!
u rel 9Dd The temperature and mass correction functions FT and FM,j are
Red ¼ ð8Þ calculated as
mg
In order to calculate the temperature Tid of the droplets, it is ln ð1þ BÞ
FðBÞ ¼ ð1 þ BÞ0:7 ð17Þ
necessary to calculate the heat and mass transfer rate to account B
for both the convective and latent heat loss of the droplets. The using BT or BM,j for FT and FM,j, respectively. In the relation for the
energy conservation equation for each parcel of droplets under temperature correction function FT, BT is the Spalding heat
the assumption of a uniform droplet temperature is (AVL, 2008): transfer number defined as
dTid BT ¼ ð1 þBM Þf 1 ð18Þ
mid cp,d _ iE þ Q_
¼ LðTid Þm ð9Þ
dt
cp,d Sh 1
Here, cp,d is the mean specific heat capacity of the droplets (i.e., an f¼ ð19Þ
average over all components in the droplet), L(Tid) is the latent cp,g Nu Le
heat of evaporation (assumed to be a function of the droplet Here, cp,g is the gas phase specific heat capacity at reference
temperature) and Q_ is the heat transfer rate between the conditions and Le is the Lewis number. Finally, the heat transfer
surrounding gas and the droplets. As the spray consists of a rate Q_ between the droplet and the gas phase for the whole parcel
5704 D. Suzzi et al. / Chemical Engineering Science 65 (2010) 5699–5715

is defined as
 
c ðT T Þ
_ iE p,d 1 id LðTid Þ
Q_ ¼ m ð20Þ
BT
Mixture fractions and mixture properties for each component j
at the drop surface needed in Eq. (12) are calculated using the
activity coefficients gj:
pv,j
xj,s ¼ xj,L gj ð21Þ
p
Here, xj,s and xj,L are the mole fraction of species j in the gas
and liquid phase, respectively. Note, that the mole fraction xj,s is
directly related to the mass fraction wj,s that is used in the
calculation for the mass transfer rate. pv,j is the vapor pressure of
pure species j and p is the total pressure. Instead of using Raoults’
law, i.e., assuming gi to be equal to 1, the activity coefficients used Fig. 3. Droplets/wall deposition model: critical curve.

in our work have been calculated using a group contribution


method (UNIFAC method, Peres and Macedo, 1997). This is in line Furthermore, we do not take into account the exact shape of
with the work of Attarakih et al. (2001), which described water– the liquid film and assume a planar film surface on the tablet. This
glycerol mixtures using the UNIFAC method and used the Antoine assumption is supported by the fact that (i) the characteristic time
equation to describe the temperature-dependency of the vapor of drop spreading ts is of the order of (Rrim/Dd)10mLDd/sL (Rrim)
pressure. being the characteristic rim radius, Yarin, 2006), and hence, is
In summary, the calculation of the mass transfer rate m _ iE,j for very small for the small droplets considered in our work and (ii)
each species and the heat transfer rate is performed using the the tablet will be quickly covered by a film with a thickness in the
following procedure: order of a few droplet diameters (see Fig. 10).
According to the local properties of the impacting droplets
 calculate the mass fraction wj,s of each species j at the surface either the liquid mass is transferred to the wall film (deposition)
of the droplet (Eq. (21)), or new particles are generated (splashing regime), which rebound
 calculate all physical properties at the reference conditions, away from the tablet surface. Specifically, the secondary droplets
 calculate Nu0 and Sh0, could then
 calculate BM,j, FM,j, Shj and the mass rate of change for each
species from Eqs. (12), (16) and (17), as well as the total mass  evaporate and not deposit (i.e., spray drying effect),
transfer rate from Eq. (10),  deposit on the coater wall,
 evaluate the Spalding heat transfer number BT (Eq. (18)), the  exit the coater with the exhaust air, or
corrected Nusselt number Nun (Eq. (16)) as well as the total  deposit on another tablet.
mass transfer rate from the energy balance (Eq. (13)),
 compare the total mass transfer rates from Eqs. (9) and (13) In our study we neglect the last option. The flow path of these
and correct the heat transfer number BT until both total mass droplets can only be analyzed using a detailed simulation of the
transfer rates are equal, air flow inside a coater. This will be part of a future study.
 evaluate the heat transfer rate from Eq. (20). As we have a binary mixture of glycerol and water, the
physical properties of the droplets (i.e., density, surface tension
The presented simulations are performed with a two-way and viscosity) are a function of the local composition and
coupling between the continuous and the discrete phases, i.e., all temperature. In our work we have taken this information from
source terms for mass, momentum and energy can be also found tabulated values from a manufacturer’s specification (The Dow
in the transport equations for the gas phase. Chemical Company, 2009) using linear interpolation.

4.2. Droplet impact 4.3. Wall film model

The numerical model describing the interaction between The deposition, flow and drying of the coating solution on a
impacting droplets and the wall (i.e., the tablet surface) is based tablet is critical for the quality of the tablet coating. In order to
on the work of Mundo et al. (1995). Splashing or deposition occur predict the distribution of the coating solution on the tablet, it is
depending on the dimensionless droplet Reynolds and Ohnesorge necessary to model the flow of the deposited fluid film. Some
numbers, defined as general theoretical models to describe film formation and its flow
rL vd? Dd mL on objects are available in literature (e.g., Yih, 1986; Baumann and
Re ¼ , Oh ¼ pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi ð22Þ
mL rL sL Dd Thiele, 1990). However, they are still not used in the pharmaceu-
tical coating technology. In our work, we tried to adopt some of
The (empirical) critical curve delimiting the splashing and
these models for the prediction of film formation on tablets using
deposition regimes is shown in Fig. 3 and can be expressed as
the modeling assumptions described in the next chapter.
Ohcrit ¼ 57:7 Re1:25 ð23Þ
The ratios of the incoming and outgoing tangential and the 4.3.1. Model assumptions
normal velocities are also included in the spray-wall interaction Due to the high viscosity of the coating solution compared to
model, leading to empirically determined ratios of 1.068 and the surrounding air, the fluid film is only slowly flowing over the
0.208 for smooth walls, respectively. This critical curve is valid for tablet. In addition, evaporation of volatiles from the film, as well
the impact of single droplets, i.e., we neglect droplet–droplet as heat transfer from and to the surrounding gas are major factors
interactions during the impact. Since the mass loading of droplets impacting that distribution of the film. In order to obtain a
is relatively low, this assumption is expected to be valid. detailed but computationally still tractable prediction of the film
D. Suzzi et al. / Chemical Engineering Science 65 (2010) 5699–5715 5705

behavior, we make the assumption of a relatively thin film, i.e., that the film created by these droplets is uniform and is well
the film thickness is much smaller ( o500 mm) than the described with a mean film thickness. This allows us also to use a
characteristic dimensions of the simulated domain. For film two-dimensional flow model for the film spreading (see the next
coating processes this assumption is valid, as the final coating section). Furthermore, we have assumed the tablet to be non-
layer thickness is typically in the range of 100 mm. It can be porous, i.e., the coating suspension cannot penetrate into the
expected that the film thickness will be of the same order of tablet. Also, we take into account the change of the liquid-phase
magnitude. Following this assumption, the volume of the film can density and viscosity due to temperature or composition change.
be neglected and no adaptation of the computational grid is The spreading of the wall film around the edges of the tablet land
necessary. Furthermore, the film surface can be assumed to be is highly important for the coating quality. Anyhow, the high film
parallel to the solid wall. Thus, the wall film is modeled as a curvature and the deriving surface tension effects would only
two-dimensional layer with a spatially distributed thickness d. locally affect the transport equation for the wall film in a tiny
Due to the small dimensions and the small velocity of the film, fraction of the total surface area. Thus, we neglect the effects in
interfacial shear stresses and wall friction influence the film much this area.
more than inertial forces and lateral shear (see Cebeci and
Bradshaw, 1977). For this reason, we have neglected these effects 4.3.2. Governing equations
in the momentum conservation equation of the wall film, In this section, the governing equations that are used to model
significantly reducing computational costs. When neglecting the above effects are described. Other aspects, e.g., such as the
inertial forces we assume that the film is at a steady state. Thus, numerical discretization or alternatives to the models used in
the velocity profile of the film is instantaneously determined by our work, can be found in the user guide of the software used
the forces acting on the wall film. In this work, the following (AVL, 2008).
effects have been taken into account: Here we introduce the film thickness equation, which
represents the basic governing law for the wall film flow. It is a
 the stress induced by the surrounding gas flow on the liquid modified formulation of the continuity equation for the liquid
film, i.e., the interfacial shear stress, as well as the pressure phase on the tablet and is presented here for a Cartesian
gradient induced by the surrounding gas; coordinate system:
 body forces, i.e., gravitational acceleration;
@d @du1 @du2 1
 multi-component evaporation from the film, taking into þ þ ¼ sm ð24Þ
account individual diffusion coefficients of each component
@t @x1 @x2 r
in the gas phase; The terms d and r represent the thickness and the density of the
 interaction with impinging droplets, i.e., deposition of the wall film, sm is the area-specific mass source term for the liquid in
coating solution on the film, as well as the change of droplet the wall film. Since in our case the wall (i.e., the tablet surface) is a
size due to splashing on the droplet (Mundo et al., 1995). This closed surface, no boundary conditions (BCs) but only initial
effect has already been detailed in Section 4.1 of this paper. conditions (ICs) are needed, i.e., zero film thickness at time zero.
Eq. (24) can be solved in a straightforward manner once the source
The impact of film deformation on the interaction between the term sm (due to deposition of droplets on the tablet and evaporation
gas phase and the film (momentum, heat and mass transfer) is from the film) and the mean velocity components u1 and u2 are
taken into account via empirical models for the ‘‘equivalent sand known. The source term sm is known from the spray solution as
grain roughness’’ of the film. In addition, we solve the enthalpy described in Section 4.1 of this paper. The mean velocity
equation of the wall film in order to predict its temperature, i.e., components u1 and u2 are calculated from a momentum balance
we take into account conductive and convective heat transfer, as of the liquid film. In our work we use an analytical solution for the
well as latent heat effects due to evaporation. In our model we wall film’s momentum equation, which is motivated by the
assume laminar flow behavior. This hypothesis is acceptable as assumptions made above. Thus, the momentum equation reduces
!
turbulence occurs only at large Reynolds numbers not obtained in to a balance of the shear stress imposed on the film t I and the
the film. Film entrainment, i.e., the re-dispersion of the wall film viscous and turbulent dissipation within the film (see Fig. 4)
into the gas flow via detachment of droplets from the film, does !
t ðyÞ !
@u
not play a significant role in our application and is therefore ¼ ðn þ e m Þ ð25Þ
r @y
excluded. The droplet spreading after the impact at the tablet
surface is accounted for in the statistics of the Lagrangian DDM
method. The hypothesis of parcels containing a certain number of
real droplets leads to the assumption that the droplets impacting
on a tablet mesh face homogeneously distribute on it. The average
number of real droplets in such a parcel is in the order of a few
thousand (for the parameters as per Table 1). Thus, we assume
wall
Table 1 film’s
Basis set (B) of the simulation parameters.
surface
Parameter Symbol Value

Droplet diameter Dd 20 mm y
Droplets injection velocity vd 15 m/s
Gas temperature Tg 298.15 K
Droplets temperature Td 298.15 K wall
Tablet temperature TTAB 298.15 K (tablet)
Total injected mass Minj 0.1 g x
Injection time tinj 0.1 s
Mass fraction of glycerol in water w 20 wt%
Fig. 4. Stress and velocity distribution in the wall film.
5706 D. Suzzi et al. / Chemical Engineering Science 65 (2010) 5699–5715

P
Here, m denotes the turbulent eddy viscosity within the frame- The integration of Eq. (27) for turbulent flows (i.e., em a0)
work of Boussinesq’ hypothesis for the description of turbulent requires the definition of the eddy viscosity em as a function of the
! !
dissipation. t ðyÞ and u represent two-dimensional vectors in the dimensionless wall distance y + . However, since the film flow
plane of the wall for the shear stress and the velocity, respectively. remains laminar in our work, this is not discussed here.
Both depend on the wall-normal coordinate y. Clearly, the local In the momentum equation (see Eq. (25)) for the film flow,
!
distribution of the shear stress t ðyÞ uniquely defines the shape of surface tension effects near the front of the film have been
P
the velocity profile in the film once the turbulent eddy viscosity m neglected, since these effects (i) will be limited to the front of the
is known. film, as the curvature of the film is significant only in this region,
!
The interfacial shear stress t I induced by the gas flow, the (ii) we assume that the coating solution wets the surface, and
!
component of the gravitational force g 99 parallel to the wall, as thus, spreading is governed by viscous flow as the curvature at the
well as the longitudinal pressure gradient @p=@x determine the edge of the film is small. Furthermore, a rough estimate of the
distribution of shear stress across the film, given by capillary number (mLV/sL) (for mL ¼10  2 Pa s, sL ¼7  10  2 N/m,
  V¼30 m/s) yields a quantity b1, indicating small surface tension
@p
!
t ðyÞ ¼ r! g 99 
!
ðdyÞ þ t I ð26Þ effects. However, in regions where the characteristic film velocity
@x
V is low, the capillary number is small and surface tension may
!
The calculation of the interfacial shear stress t I is non-trivial, influence film spreading. In order to take into account
as the interfacial stress itself influences the flow of the gas over surface tension and contact angle effects, a detailed resolution
the film due to the deformation of the phase boundary. In our of the front of the film is necessary. This will be considered in
!
work, this effect is taken into account by calculating t I using an further studies.
approximation of the velocity profile in the gas phase, i.e., the so- Next, we describe the enthalpy equation for the wall film to
called wall functions, with coefficients that depend on the wall obtain the film temperature distribution on the tablet. The
shear stress and on the film thickness. In essence, we model the simplest approach would be to assume that the film has the
deformation of the film surface by a correlation for the equivalent same temperature as the tablet. This is only valid, if the film is
sand grain roughness ks as a function of wall shear stress and film very thin and heat transfer between tablet and film is very fast. In
thickness. ks is then used to calculate a characteristic Reynolds our work, we assume that the gas phase, the wall film and the
number, and finally we can correlate this Reynolds number with wall (i.e., the tablet) have different temperatures. Assuming a
the coefficients in the wall function. Due to this complex homogeneous film temperature over the film thickness, the
interaction between film flow and interfacial shear stress, it is enthalpy equation for the film can be written as
necessary to iteratively solve for the mean film velocity, as  
detailed below. Details of this calculation can be found in AVL @h !
rd þ rUðh u Þ ¼ ðh_ S,fw h_ S,fg m
_ E hE þ h_ S,imp þ h_ S,ent Þ ð29Þ
(2008). @t
!
To obtain the velocity profile in the film, we first transform u
The first two terms on the right hand side of Eq. (29) represent
and y in Eq. (25) into dimensionless
pffiffiffiffiffiffiffiffiffiffiffiffi coordinates by introducing
the heat fluxes in W/m2 between film and wall, and between film
the friction velocity ut ¼ tW =r (see, for example, Holman,
and the gas phase, respectively. In our work, these terms are
1989). Here, tW is the wall shear stress, i.e., the stress at y ¼0.
!þ ! modeled using appropriate correlations for the Nusselt number,
Thus, we define the dimensionless wall film velocity u ¼ u =ut
i.e., predictions for the heat transfer coefficient based on
and the dimensionless wall distance y ¼ yut =n.
þ
experimental data have been used. Also, the temperature of the
Hence, we obtain
wall, i.e., the tablet, has been assumed to be uniform. The third,
!þ ! þ fourth and fifth term on the right hand side of Eq. (29) denote the
@u t ðy Þ=tW
¼ ð27Þ enthalpy change due to evaporation (m _ E is the evaporation mass
@y þ 1 þ em =n
flux in kg/(m2 s)), the area-specific enthalpy transfer from spray
This equation represents a general formulation of the film flow, droplet via impingement and the area-specific enthalpy loss from
both for turbulent and laminar films, with or without gravity, droplet entrainment, respectively.
interfacial shear or pressure gradients. In case of laminar flow, Similar to the film thickness equation, the enthalpy equation is
where em is equal to zero, the integration of Eq. (27) leads to an solved by using the result of the simplified momentum equation
analytical solution for the dimensionless velocity profile (see, for !
for u , i.e., Eq. (28).
example Prandtl et al., 1990). In our case, we assume a laminar Finally, the total evaporation mass flux m _ E from the film
flow of the wall film. This assumption is justified by the fact that has to be modeled. The evaporation process can be described by
in our simulations the wall shear stress and the film thickness are Stefan’s law of unidirectional diffusion, which is used in our
significantly below 1.2 Pa and 0.2 mm, respectively, values for work, i.e.,
which a transition from laminar to turbulent flow has been
  
observed in the literature for internal combustion engines rb @wj
_ E,j ¼  g g,j
m ð30Þ
applications (AVL, 2008). By integrating over the film thickness, 1wI,j @y I
we obtain the mean film velocity u for laminar flow:
    Here, rg is the density of the gas phase, Dj,2 is the molecular
! d ! dp !
u ¼ 2d r g 99  þ3 t I ð28Þ diffusion coefficient of the evaporating species j in the gas, wI,j is
6m dx
the mass fraction of each evaporating species j at the interface and
Eq. (28) is used in the film thickness equation (Eq. (24)) to ð@wj =@yÞI is the gradient in wall-normal direction of the mass
solve for the time evolution of the film thickness. We stress once fraction at the interface. rg, Dj,2 and wI,j can be calculated from the
more, that due to the assumption of negligible inertial forces the ideal gas law, empirical correlations and the saturation pressure,
mean film velocity adapts instantaneously to the stresses acting respectively. However, the gradient of the mass fraction at the
on it. The film velocity is, however, transient due to the inherently interface depends on the local flow conditions and is therefore not
instationary flow of the surrounding gas flow resulting in an known. In our work we use the analogy to the turbulent velocity
instationary interfacial stress. Also, the mass, and consequently profile to approximate this gradient, taking into account the
the thickness of the wall film, change with time due to droplet rough surface of the wall film. Details of this model can be found
deposition and evaporation of the coating solution. in AVL (2008).
D. Suzzi et al. / Chemical Engineering Science 65 (2010) 5699–5715 5707

5. Results This experimental method is capable of simultaneously measur-


ing diameter, velocity and mass flux of the injected spray droplets.
5.1. Base case definition The chosen nozzle was a Schlick 930Form 7-1 S35 ABC, typically
used for pharmaceutical coating processes. Atomizing air (AA) and
As mentioned above, our goal was to investigate the influence pattern air (PA) were both set equal to 1.2 bar, leading to an
of different operating parameters on the film formation on coated injected mass flow of approximately 60 g/min. The distribution of
tablets. In order to define a realistic base set of parameters for our droplet diameter and velocity at a distance of 200 mm from the
simulations, experimental investigations of a spray gun via Phase nozzle tip are shown in Figs. 5 and 6, respectively. These average
Doppler Anemometry (PDA) technique have been performed (for values were obtained by scanning the spray along a line
the technique refer to Hirleman (1996), the measurements have perpendicular to the spray axis. As well known in the literature,
been performed by us at Duesen-Schlick GmbH, Germany). real sprays have a range of drop sizes and velocities, which will
greatly influence their trajectories, their interaction and influence
on the turbulent gas flow, evaporation time, likelihood of
bouncing, and degree of coverage on the tablet’s surface. In
order to understand in detail the behavior of different droplet
sizes and velocities, we considered variations of mono-disperse
droplet population in order to quantify the singular effects of
diameter and velocity variations. Mono-dispersed droplets size of
20 mm, as well as an initial velocity of 15 m/s was selected as a
base case, which is a good compromise between the volume- and
number averaged data in Figs. 4 and 5. The temperature in the
computational domain was initially set to room conditions
(i.e., 298.15 K). The base set of parameters is defined in Table 1.
As already discussed in Section 4.1, these values are the initial
Fig. 5. Phase Doppler Anemometry (PDA) measurements of droplets size
conditions of a few centimeters downstream the nozzle outlet
distribution (average values 200 mm from the nozzle tip). where secondary atomization, collision and coalescence become
insignificant. Standard values for the physical properties of the air
and water have been used. The physical properties (viscosity,
density) of the glycerol–water mixture have been taken from the
manufacturer’s specifications (The Dow Chemical Company,
2009).
A hybrid three-dimensional computational grid has been
generated with a structured wall layer around the tablet (see
Fig. 7). This structured wall layer is three cells in depth in order to
sufficiently resolve the wall-near region. The computational grid
consisted of a rectangular box with a cross section of
0.18 m  0.18 m and a length of 0.25 m. The spray nozzle was
located at the upper part and in the center of the box. The distance
between spray nozzle and the object (granule, tablet) to be coated
has been set to 15 cm, which is a realistic value in industrial
Fig. 6. Phase Doppler Anemometry (PDA) measurements of droplets velocity practice. Typically, round convex tablets were used in our work.
distribution (average values 200 mm from the nozzle tip). The tablet’s main diameter was chosen to be 10 mm, and the

Spray nozzle

150 mm
Droplets

Tablet

Fig. 7. Simulation domain and section of the 3D-hybrid computational mesh.


5708 D. Suzzi et al. / Chemical Engineering Science 65 (2010) 5699–5715

height-to-diameter ratio was set to 0.67:1. The band thickness r21 and r32, the values of the key variables f, the approximate
and the cap radius of curvature were equal to 3 and 7.6 mm, relative error e21 21
a , the extrapolated relative error eext, the
respectively. The box was modeled to be open on top and bottom, extrapolated solution f21 ext and the fine-grid convergence index
in order to allow for a gas flow induced by the injected liquid GCI21
fine are shown in Table 2. According to these results, the film
spray. In our work we oriented the top surface of the tablet thickness appears nearly equal for the finest and the middle mesh,
perpendicular to gravity and to the incoming droplets. The effects leading to a deviation of only 0.020%. Thus, mesh 2 was used for
of different tablet orientations with respect to the spray, as well as further simulations. Note that the GCI method accounts only for
the impact of different tablet bed angles (and thus gravity) will be discretization errors and not for modeling errors.
part of future work. A typical example of our results is presented in Fig. 8. The initial
In order to test the mesh quality and the convergence of the choice of pure water leads to increased wall film evaporation
numerical simulation, preliminary test runs have been performed compared to realistic cases. The evaporation process mainly takes
for pure water droplets and continuous spray injection. Based on place in the upstream part of the tablet, indicated by the low film
these results a computational time step of 1  10  4 s was shown thickness and the significant accumulation of water vapor near the
to be adequate in order to describe all the important scales of the upper edge of the tablet. Clearly, evaporation as well as the flow of
process. The convergence criteria for the residuals have been the film induced by the interfacial shear stress seems to surpass the
chosen as 1  10  4 for momentum, turbulence and species accumulation of water by droplet deposition in this region of the
conservation equation, and 1  10  6 for the energy conservation tablet. Furthermore, it can be seen from Fig. 8 that the evaporated
equation. A grid dependency study has also been performed to water is transported along the cylindrical part of the tablet into the
assess the quality of the computational mesh. For this purpose we wake region of the flow. Accumulation of water vapor is highest
used the well-accepted Grid Convergence Index (GCI) from near the cylindrical part of the tablet, whereas water vapor
Roache et al. (1986). Three meshes made of 15,527, 3884 and accumulation in the wake region is less pronounced. In both
1205 face cells on the biconvex tablet surface, respectively, called regions, i.e., in the wake and the cylindrical part, the high vapor
mesh 1, mesh 2 and mesh 3, were used. The average film concentration leads to a decreased evaporation rate, resulting in
thickness f after 0.25 s has been chosen as the key variable for the locally higher film thicknesses. It should be noted that in a ‘‘real’’
GCI study. The face cells numbers N, the grid refinement factors tablet bed a single tablet is not suspended in space and the wake
would be significantly different (or even not present). Hence, the
results for the rear part of the tablet may change significantly.
Table 2
Nevertheless, the goal of our study was to compare the effects of
GCI calculation of discretization error. different process parameters on the film formation process. Thus,
the major aim was to analyze the droplets collision and the film
Parameter Symbol Value spreading on the surface of the singular tablet. A more detailed
reproduction of the tablet bed environment was included in further
Face cells number N1; N2; N3 15,527; 3884; 1205
Grid refinement factor (mesh 2 to 1) r21 2.0 analysis.
Grid refinement factor (mesh 3 to 2) r32 1.8 Furthermore, our analysis describes only one pass of a tablet
Average film thickness (mesh 1) f1 1.606e  4 m through the spray zone at a defined angle with respect to the
Average film thickness (mesh 2) f2 1.596e  4 m
spray. In a real system, tablets will enter the spray zone multiple
Average film thickness (mesh 3) f3 1.370e  4 m
Extrapolated solution 1.60626e  4 m
times at different angles, thus resulting in a statistical distribution
f21
ext
Approximate relative error 0.62%
of the coating layer. Nevertheless, the presented analysis is
e21
a
Extrapolated relative error e21 0.016% important as it details under which conditions a uniform layer can
ext
Fine grid convergence index GCI21 0.020% be achieved and how the operating conditions impact the coating
fine
process.

Fig. 8. Simulation with water droplets. Color code in the gas phase denotes water vapor mass fraction. Color code on the tablet denotes film thickness.
D. Suzzi et al. / Chemical Engineering Science 65 (2010) 5699–5715 5709

5.2. Variations over the sphere and the tablet. Thus, the transport of the liquid
phase on a tablet to be coated is substantial, and it is important to
In a second step, the main parameters of the base set have model this part of the process. In our simulations the spreading of
been modified and a glycerol–water mixture has been used in the film is mainly influenced by the stress from the gas phase, the
order to mimic a realistic coating process. Two different tablet momentum introduced by the impacting droplets and by gravity
shapes have been considered, i.e., a sphere and a convex tablet to a smaller extent. The eventual tumbling of the tablet is not
with the main diameter equal to 10 mm. Furthermore, following taken into account in the current work.
parameters has been varied: The results in Figs. 8 and 10 show that the film thickness
reaches 70 and 100 mm already after a single ‘‘pass’’ in the spray.
 droplets diameter Dd, However, as discussed in the introduction, typical film thick-
 environmental gas temperature Tg, nesses after an entire coating operation are less than 100 mm. The
 droplets injection velocity vg, explanation is that the typical film thickness refers to a solid film,
 glycerol mass fraction in the coating solution w. whereas in our simulations the film thickness in a single ‘‘pass’’
refers to a liquid film with suspended polymers. Thus, the drying
process is not completed and the film mainly consists of the liquid
In order to reduce the amount of simulations, only one variable
components.
has been varied at once, resulting in the variation stars shown in
According to the results in Fig. 10, the spreading of the film
Fig. 9. Simulations have been performed for a total time span of
seems to be completed after approx. 0.4 s for the base conditions
0.5 s, whereas the injection of droplets stopped after 0.1 s. This
in our study. As can be seen, even the shape of the coated object
choice was motivated by typical tablets velocities and residence
strongly influences the film thickness distribution as well as the
times in the spray zone of industrial coaters, as described by
total mass deposited. For example, in case of the tablet, a
Kalbag et al. (2008) and also discussed in Section 2.2 of this paper.
significant higher amount of droplets deposit on the surface
leading to a substantially higher film thickness. Also, the location
5.3. Analysis of the results of the maximum film thickness after 0.5 s is different for the
sphere (hmax at a polar angle of approx. 1201) and the tablet
Fig. 10 shows the transient behavior of the film formation (hmax at the backside of the tablet).
process for both the sphere, as well as the tablet. Clearly, during In the following section, results for different cases are
the injection of droplets for 0.1 s they primarily deposit at the presented at a spray time of 0.5 s. The curves shown in Figs. 11
front of the surface to be coated. However, after the injection has and 12 represent the cumulative frequency distributions of
stopped (t ¼0.1 s), the film is more or less uniformly distributed the local film thickness for all the cases in both variation stars.

Fig. 9. Variation star for sphere (left) and tablet (right). The base case conditions (B) are specified in Table 1.

Fig. 10. Time evolution of the film at different time steps for a sphere (top) and the tablet (bottom) for the base conditions (Table 1).
5710 D. Suzzi et al. / Chemical Engineering Science 65 (2010) 5699–5715

because the cumulative frequency distribution has the smallest


initial slope.
For the tablet (results shown in Fig. 12), the situation is
different and cases 1, 4 as well as 5 indicate significant effects on
the film thickness distribution. Same as for the sphere, the larger
droplet diameter (case 1) results in a much lower deposition of
droplets on the surface. This is caused by splashing and rebound
of the droplets from the tablet’s surface. In addition, a significant
part of the tablet’s surface is not covered, indicated by a value of
approx. 0.26 for the first class of the cumulative frequency
distribution. Case 4 (i.e., a droplet velocity of 30 m/s compared to
15 m/s of the base case) shows mainly two effects on the film
thickness distribution: (i) the film thickness after 0.5 s is only a
fraction of that obtained in the base case as indicated by the shift
to the left of the distribution. This is due to splashing of droplets
Fig. 11. Cumulative frequency distribution of the local film thickness of the coated on the tablet; (ii) the coating quality decreases as there exist
sphere at t¼ 0.5 s (for the base case B defined in Table 1 and the variations in regions that are completely free of liquid. This is again indicated
Fig. 9). by a high value for the first class in the cumulative frequency
distribution for case 4 in Fig. 12. Finally, case 5 (higher glycerol
content of the liquid phase) shows similar trends, i.e., a slightly
reduced film thickness, as well as decreasing coating uniformity.
The decreased film thickness for the higher glycerol content can
be attributed to a change in physical properties of the droplets
(density, viscosity and surface tension) resulting in a reduced
deposition on the tablet. The decreasing coating quality is due to
the higher viscosity of the coating film, resulting in lower mean
film velocities on the film. Consequently, the film cannot spread
as quickly as in the case of lower glycerol concentration. The
optimal conditions with respect to the coverage of the surface
with the film seem to be case 3, as here the initial slope is
smallest. However, also the base case, as well as case 2, indicate
acceptable coverage of the surface with the coating solution.
The time evolution of the total film mass on the tablet is shown
in Fig. 13. A total of 100 mg has been injected, of which only a
fraction impacts on the tablet’s surface. 80 mg of the total mass
Fig. 12. Cumulative frequency distribution of the local film thickness of the coated are water and 20 mg are glycerol, the latter having a very low
tablet at t ¼ 0.5 s (for the base case B defined in Table 1 and the variations in Fig. 9). vapor pressure, leading to a significantly lower evaporation rate
compared to water. In the base case approximately 9.4 mg of the
coating liquid are deposited after 0.15 s. In the following, the film
These plots have been derived from the simulation results by mass starts to decrease, due to the fact that the injection of
defining classes for the film thickness and allocating the fraction droplets is stopped and evaporation of the film starts. After 0.5 s
of the surface that fits into these classes. Thus, the cumulative the film mass has nearly linearly decreased to 8.4 mg ( 10%),
frequency distribution represents the fraction of surface area that indicating an almost constant mean evaporation rate. Compared
is covered with a film with a thickness lower or equal than a to the base case, the bigger droplets (case 1) appear to deposit
certain value. A wide distribution of the film thickness on the consistently less than the smaller ones, resulting in a peak value
surface, i.e., poor coating uniformity, is indicated by a small slope of only 0.85 mg for the total film mass after 0.12 s. This can be
of the curve. On the contrary, a narrow distribution, i.e., a good explained by the significantly higher Reynolds number of the
coating uniformity, is indicated by a steep increase of the curve. impacting droplets (case 1 leads to a 2.5-fold increase in the
Concentrating on the case for a sphere (Fig. 11), we see that the Reynolds number, but only to a 37% decrease in the Ohnesorge
base case, as well as the cases 2–5, behave similarly and do not number), which leads to the occurrence of splashing. Also, the
show significantly different mean wall film thicknesses. In
contrast, case 1 (droplet size increase from 20 to 50 mm) shows
a significantly lower mean wall film thickness. A significant
fraction of the surface does not seem to be covered by liquid at all.
This is indicated by the fact that the first class of the cumulative
frequency distribution has a value of approx. 0.37, i.e., 37% of the
surface have a lower film thickness than the first class that has
been analyzed. Looking at the shape of the distribution, it can be
seen that for the base case, as well as for the cases 3–5, the
distribution is bimodal, i.e., the distribution shows two regions
with a local maximum in the slope. Such a bimodal distribution
indicates that there exist zones with substantial different film
thicknesses. In summary, only the increase in droplet size (case 1)
results in a significant decrease in spray deposition, consequently
leading to uncoated spots on the surface. The best conditions with Fig. 13. Time evolution of the film mass on the surface of the coated tablet (for the
respect to surface coverage by the film are realized in case 2, base case B defined in Table 1 and the variations in Fig. 9).
D. Suzzi et al. / Chemical Engineering Science 65 (2010) 5699–5715 5711

time profile of evaporation for case 1 is significantly different


from that of the base case. As can be seen from Fig. 13, after the
peak value of the film mass has been reached in case 1,
evaporation takes place at a relatively high rate, until the film
mass has been reduced to 0.39 mg, i.e., half of the peak value, after
approx. 0.2 s. At this point the evaporation rate reduces
significantly due to the fact that glycerol mass fraction
increased (water is evaporating first due to the higher vapor
pressure from the glycerol–water mixture). This results in a
decrease of the vapor pressure of the film liquid, causing a
pronounced decrease in the evaporation rate. The final film mass
is 0.32 mg, i.e., the total loss of film mass in the second phase of
the evaporation of the film is marginal. Comparing the base case
with case 4, i.e., a higher droplet velocity, we observe a similar
shape of the time profile for the total film mass as in case 1: In Fig. 14. Mean film thickness on coated sphere (left bars) and tablet (right bars) at
case 4 the peak value of the film mass is significantly less (4.4 mg t¼ 0.5 s (for the base case B defined in Table 1 and the variations in Fig. 9).
after 0.14 s) compared to the base case. This is again due to
splashing, as the Reynolds number of the droplets is again higher
than in the base case. Also the evaporation rate of the film on the This factor is the fraction of tablet surface that are not covered
tablet is significantly higher due to the higher gas velocity by the coating film.
induced by the higher droplet velocity. This leads to a nonlinear Based on these indicators, other parameters may be derived to
time profile of the film mass caused by the accumulation of assess the coating quality. For example, the relative standard
glycerol in the film, because a significant fraction of the water has deviation of the coating thickness can be easily obtained by
already evaporated. In summary, the total loss of film mass after dividing the mean value by its variance. In Fig. 13 we have already
0.5 s for case 4 is 2.3 mg or 52% due to evaporation, which is discussed the rate of change of the total film mass for a tablet, a
significantly more than in the base case. Thus, the tablets are quantity which is directly proportional to the mean film thickness
already relatively dry after 0.5 s. introduced in this section. Here we focus once more on the
The presence of more glycerol in the coating solution (case 5) comparison of the mean film thicknesses obtained for different
leads to (i) a lower level of film mass on the surface, as well as to cases. However, we also include the results for the coated sphere
(ii) a significantly lower mean evaporation rate from the film. The (see Fig. 14). As can be seen, in the base case, as well as in cases 2,
initially deposited droplet mass is 7.3 mg after 0.15 s, whereas the 3 and 5, the mean film thickness is significantly lower for the
final film mass after 0.5 s is 7.1 mg (  2.7%). The first effect, i.e., sphere compared to the tablet. This indicates that under the
the lower level of film mass, can be explained by the change of the droplet deposition parameters defined in the base case (which
physical properties (i.e., density, surface tension and viscosity) of essentially do not change in the cases 2, 3 and 5), the sphere
the spray droplets, such that the deposition rate is decreased. The receives consistently a lower amount of coating liquid, i.e., sphere
second effect, i.e., the reduced evaporation, is again due to the and tablet behave similar and are nearly unaffected by
lower vapor pressure in case of a higher glycerol mass fraction in temperature and viscosity of the coating solution. This indicates,
the film liquid. as already mentioned in the discussion of Fig. 13, that the
Case 2 (higher temperature) does not show a strong effect on increased evaporation rate due to a higher temperature does not
the total film mass time profile. Obviously, the coating process is play a significant role under the conditions used in this work.
not very sensitive with respect to small changes in the gas However, when changing droplet size (case 1) or droplet velocity
temperature, i.e., the evaporation rate seems unaffected. Also, for (case 4), the sphere receives more coating solution compared to
case 3 (significantly higher gas temperature) the evaporation rate the tablet. This change is thought to stem from a regime change
is only slightly increased (evaporation loss of 1.3 mg compared to from droplet deposition to splashing. Obviously, in the case of
1.0 mg in the base case after 0.5 s). Thus, even the wide range of spheres the deposition is significantly less reduced in the
gas temperatures does not significantly alter the time evolution of splashing regime compared to tablets. We believe that this
the total film mass present on the tablet. behavior is due to the differences in the separation behavior of
the gas flow. The gas flow is aligned longer with the sphere’s
surface, and droplets generated by splashing have a second
chance to deposit. For the tablet, the flow separates early, i.e., at
5.4. Assessment of the coating quality
the beginning of the cylindrical region, and droplets are less prone
to impact a second time. Hence, we conclude that the mean film
In order to analyze the coating quality, i.e., the homogeneity
thickness deposited on a given surface depends mainly on its
and the uniformity of the obtained film, the following quality
shape (e.g., we observe an almost 50% decrease in the case of a
indicators have been analyzed:
sphere compared to the tablet for case 3) as well as the impact
parameters (Re, Oh) of the droplets. The solution’s viscosity, as
 mean film thickness (hmean), well as the air temperature, show only minimal effects on the
 variance of the film thickness on the surface (s2), mean film thickness.
 delta (d), defined as the quotient of the maximum (hmax) and In Fig. 15 we analyzed the film thickness variance on coated
the mean (hmean) film thickness value: sphere and tablet. We observe that we have a similar situation as
hmax for the mean film thickness. Thus, the variance is lower for the
d¼ ð31Þ sphere compared to the tablet for cases B, 2, 3 and 5, i.e., in the
hmean
case where almost no splashing occurs. This clearly indicates that
According to this definition a perfectly homogeneous film the coating solution can flow more easily over the regularly
would have a d value equal to 1: shaped sphere. In contrast, the edges on the tablet make it more
 zero-thickness surface fraction (Z). difficult to obtain an even distribution of the film. In the other
5712 D. Suzzi et al. / Chemical Engineering Science 65 (2010) 5699–5715

resulting in a spot with an extremely high film thickness. Also, the


droplet size seriously influences the coating quality of the tablet,
whereas droplet velocity does not significantly alter the d value.
This is also true for the sphere.
Finally, we present Fig. 17 which shows the fraction of the
surface to be coated that has received no coating. Clearly, in those
cases where splashing occurs (cases 1 and 4) Z is between 27% and
67%, whereas for all other situations Z is below 12%. Thus,
splashing results in a significant reduction of the coverage of the
surface with coating solution and should be avoided. In contrast, a
high temperature of the gas results in a good flowability of the
film on the surface. The consequence is that nearly the complete
surface of the object is covered. This effect is very pronounced for
the tablet and less pronounced for the sphere. However, only for
case 5 (increased glycerol content) the uncoated fraction of the
Fig. 15. Film thickness variance on coated sphere (left bars) and tablet (right bars)
tablet is slightly above 10%. This indicates an almost perfect
at t¼ 0.5 s (for the base case B defined in Table 1 and the variations in Fig. 9).
coverage of the surface with coating solution in the cases without
splashing.

5.5. Shear stress distribution

The local shear stress distribution, i.e., the magnitude of the


shear stress vector in the liquid film, is shown in Fig. 18. At the
tablet edge there is a higher concentration of shear forces in
comparison to the spherical geometry. This kind of analysis could
provide important information about the quality of the tablet
layer, as different stresses during the film drying process could
possibly affect the morphology of the final film. Further studies,

Fig. 16. d value on coated sphere (left bars) and tablet (right bars) at t ¼ 0.5 s
(for the base case B defined in Table 1 and the variations in Fig. 9).

cases (i.e., 1 and 4), the sphere shows a slightly higher variance
compared the tablet. This indicates that the change to a splashing
regime reduces the importance of the flow of the liquid on the
object to be coated. In contrast to the mean film thickness where
there was almost no effect of the gas temperature, this parameter
seems to have a pronounced effect on the film thickness variance
(see cases 2 and 3, note that the y-axis has a logarithmic scale and
that case 3 has an almost 18-fold higher s2 value than the base
case!). This strong sensitivity with respect to the temperature can Fig. 17. Zero-thickness faces on coated sphere (left bars) and tablet (right bars) at
be explained by the significant change of the film’s viscosity, t¼ 0.5 s (for the base case B defined in Table 1 and the variations in Fig. 9).
which strongly decreases with temperature. Consequently, the
film can flow more easily over the tablet and can accumulate at
the rear part of the tablet’s surface, resulting in an uneven
distribution of the coating solution. However, the glycerol
content, i.e., the change of the viscosity with glycerol content at
the temperature of the base case, shows only a negligible effect. In
the cases where splashing occurs (cases 1 and 4), the variance
drops below the value for the base case. The relative variance, i.e.,
s2 =h2mean (data not shown), however, is still higher as in the base
case. This is especially true for the case of a larger droplet size,
where we observe an almost 9-fold increase of the relative
variance compared to the base case. Thus, the occurrence of
splashing seems to decrease the quality of the coating
significantly.
Similar trends are observed in Fig. 16, in which we focus on the
d value, i.e., on the ratio of maximum to mean film thickness. For
the tablet, the gas temperature has again a strong effect on the
coating quality and the influence of the glycerol content is small.
This can be interpreted by the fact that there will be an Fig. 18. Wall film stresses on the coated sphere (left) and tablet (right) at t ¼0.2 s
accumulation of coating solution at the rear part of the tablet, (base conditions).
D. Suzzi et al. / Chemical Engineering Science 65 (2010) 5699–5715 5713

both numerical and experimental, are needed to assess this coater, as the droplet properties in the spray change with the
hypothesis. Also, the mean film velocity will be higher in regions distance from the spray gun. Also, the droplet spectrum is
with higher shear stress. This will result in a locally lower film strongly influenced by the drying air flow. Hence, we stress that
thickness, i.e., regions with a higher shear stress will receive less keeping the spray-gun-to-bed distances as well as drying air flow
coating solution. This hypothesis is confirmed by our analysis of conditions in coaters unaltered during scale-up is a key factor for
the coating quality in Section 5.4, in which we already have successful industrial operation. Also, we propose that it should be
shown that a spherical geometry (with a more homogeneous possible to correctly interpret the impact of changes in produc-
distribution of the shear stress) results in a more homogenous tion-scale coaters with the aid of well designed simulations
coating film. similar to those performed in this work. For example, by knowing
the droplet size and velocity distribution of a new spray gun, it
should be possible to predict whether the film thickness and
6. Conclusions and outlook quality of the coating is seriously influenced or not.
In a realistic system the tablets will enter the spray zone
In this work we have analyzed the process of tablet spraying, multiple times at different angles. These effects have not been
as well as wetting, by means of a multiphase CFD solver. analyzed yet and will be part of future work. However, it is believed
Sophisticated models for the gas flow, droplet motion, as well as that the effects observed for a single passage of a tablet and the
for the flow of the liquid film on two different objects, i.e., a sensitivity to the process conditions will also influence coating
sphere and a convex tablet, have been developed. Using these uniformity in a typical pan coating process. As already underlined in
models we have performed a detailed variation study and Section 4.2, the splashed droplets can also bounce and deposit on
analyzed the impact of the system properties on quality attributes neighboring tablets. The effect of these phenomena will be analyzed
of the resulting liquid film. Our variation study has been designed in future works considering groups of adjacent tablets.
such as to provide a fundamental understanding of the impor- As this is one of the first studies in this field, we will validate
tance of spray parameters with respect to film formation. our simulation results with lab, as well as production-scale, data.
Our results allow the following basic conclusions: Also, we plan to introduce more complex coating solutions
containing, e.g., polymers or undissolved particles, as well as
 The shape of the object to be coated determines the gas flow non-Newtonian fluids in our simulations. Furthermore, we will
and consequently the rate of deposition, as well as heat and investigate the air flow and its impact on the spray in more detail
mass transfer. It is therefore important to take the shape of the in the future.
tablets into account when performing an analysis on the local
coating quality.
 The prediction whether deposition or splashing of droplets Nomenclature
occurs on the surface to be coated is essential for the amount
and the quality of the coating. Latin symbols
 The gas flow used in our work is strong enough to ensure that
the film liquid is covering almost the whole object during a A area (m2)
time span of 0.5 s. BM,j, BT spalding mass and heat transfer number (dimensionless)
k constant (dimensionless)
Our variation analysis showed the following trends: cp specific heat capacity at constant pressure (J/kg K)
d particle diameter (m)
 Splashing of droplets impacting on the surface dramatically D diameter (m)
reduces the total mass as well as the quality of the film. This F force (N)
may be caused be excessively high droplet velocities or large FM,j, FT mass and temperature correction functions
droplet sizes. Splashing should be in general avoided, as it (dimensionless)
leads to a lower deposition of coating solution, less surface fR fractional residence time (dimensionless)
coverage, as well as significantly higher surface roughness. The g gravitational acceleration (m/s2)
variation of droplet size showed a more pronounced effect h specific enthalpy (J/kg)
than the change in the droplet velocity. k thermal conductivity (W/(m K))
 Increasing the gas temperature does not significantly change km mass transfer coefficient (m/s)
the mean film thickness; it seriously impacts, however, the L latent heat (J/kg)
quality of the film. An advantage of a higher gas temperature is L characteristic length, length of the spray zone (m)
that the surface coverage can be increased. Also, higher m mass (kg)
evaporation rates can be expected. This and other effects n number of particles (dimensionless)
(impact on morphology) was, however, not investigated in N pan rotation rate (rpm)
detail in this work. p pressure (Pa)
 Changing the viscosity by adding more glycerol does not Q_ heat transfer rate (W)
change the mean film mass, as well as the quality attributes of R pan radius (m)
the film during film formation. sm area-specific mass source (kg/m2s)
t time (s)
Thus, we have identified the droplet diameter, as well as the tC circulation time (s)
droplet velocity, as the most critical process parameter that needs tR residence time per pass (s)
to be controlled in industrial practice. This is already well known t0 total coating time (s)
in literature (see for example Pandey et al., 2006b). However, the T temperature (K)
mechanistic understanding of these process parameters and their u, v velocity (m/s)
impact on the quality of the film has not been described until ut friction velocity (m/s)
now. Also it is clear that a simple reduction of droplet size and u+ non-dimensional flow velocity (dimensionless)
velocity at the nozzle exit could be counter-productive for a real V characteristic surface velocity (dimensionless)
5714 D. Suzzi et al. / Chemical Engineering Science 65 (2010) 5699–5715

Vmax maximum surface velocity (dimensionless) Acknowledgement


S
Vmax dimensionless maximum surface velocity
(dimensionless) We thank the reviewers for their extremely helpful comments
v fractional fill (dimensionless) with respect to tablet flow and droplet spreading on surfaces.
w mass fraction (kg/kg)
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