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12 Ansichten17 Seitenanalysis of the tablet coating process

analysis of the tablet coating process

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analysis of the tablet coating process

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12 Ansichten17 Seitenanalysis of the tablet coating process

analysis of the tablet coating process

© All Rights Reserved

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

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

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.

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.

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

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

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

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

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

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.

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

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)

x mole fraction (mol/mol)

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