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Article history: The uidized bed spray granulation process unites the steps of solid formation and product formulation in one
Received 2 September 2015 apparatus and is used to produce granulate products out of a liquid. According to different applications of
Received in revised form 3 February 2016 granules, a specic product particle size distribution is required. Thus, the ability to predict the development of
Accepted 20 February 2016
the particle size distribution is crucial for process design, optimization and scale-up. For this reason, population
Available online 23 February 2016
balance equations can be solved where the knowledge of particle size-dependent growth rates are the important
Keywords:
quantities, which are difcult to obtain by experiments.
Computational uid dynamics Using a computational uid dynamics multiphase model with one nozzle at its center, an advanced two-uid
Population balance equations model with ve uid phases is solved for short process times (~s) considering a high local and temporal resolu-
Fluidized bed spray granulation tion of the granulation process (including uid dynamics, drop deposition and energy equations) to evaluate
Industrial scale size-dependent growth rates, as a function of the current state of the process. By transferring particle growth
Particle size-dependent growth rate rates to population balance equations, the development of particle size distribution can be nally predicted for
long process times (~min).
The present work applies the predictive model to an industrial melt spray granulation process in batch mode.
Experimental data show that this model could be implemented successfully.
2016 Elsevier B.V. All rights reserved.
1. Introduction are becoming increasingly important due to the fast increase of comput-
er performance. The modeling of multiphase ows in uidized beds can
Customizing of product properties is becoming increasingly im- be divided into the EulerEuler model (two uid model: TFM) and the
portant for the production of solid particles from liquids. Fertilizer, for discrete element method (DEM).
example, must be easy to dose and dust-free to ensure a uniform dis- Using the TFM, which is proposed by Gidaspow [11], the particle
tribution on the eld and trouble-free lling without risk of dust phases are treated as interpenetrating continua. Hereby, the volume
explosion. fraction of each phase is the characteristic transport quantity. Interac-
The uidized bed spray granulation process is one possibility to pro- tions between particle phases can be modeled using the kinetic theory
duce and formulate granules out of a liquid. Thereby, a melt is atomized of granular ow [1214]. The latter has its advantage in modeling a
in a two-component jet and sprayed into the uidized bed, which con- high number of particles. Therefore, it can be used to model particulate
sists of seed particles of the same material. Droplets deposit on the par- systems in industrial applications.
ticles near the spray zone and form a lm which solidies in the cold The DEM [15] calculates the trajectory of each particle using Newto-
uidization air. Granulate products with dened particle sizes are nian equations of motion. The interactions between particles can be
formed in a step-by-step manner. modeled using spring and damper models. The gas phase is considered
Many predominant experimental research contributions on the u- as a continuous Euler phase. The DEM can consider a particle size distri-
idized bed spray granulation process have been carried out regarding bution (PSD), but is limited in the number of particles in the bed.
uid dynamics, interactions between particles and gas [13], heat trans- Coupling of computational uid dynamics (CFD) with DEM gives a
fer [4], moisture distribution [5] and growth and agglomeration kinetics good possibility to model the ow behavior of particles in uidized
[69]. Uhlemann and Mrl [10] give a good overview of process- bed systems where each particle can be tracked individually. Fries
relevant mechanisms. et al. [16] used a DEM-CFD model to describe the particle residence
The use and development of numerical simulation tools for design, time in the spray zone during uidized bed spray granulation for differ-
optimization and scale-up of uidized bed spray granulation systems ent granulator applications in batch mode. Thereby, they worked with a
specic bed mass of approximately 37 kg/m2. Heine et al. [17] also used
Corresponding author. a DEMCFD simulation to model the particle wetting in a uidized bed
E-mail address: matthias.kind@kit.edu (M. Kind). agglomerator.
http://dx.doi.org/10.1016/j.powtec.2016.02.040
0032-5910/ 2016 Elsevier B.V. All rights reserved.
P. Lau, M. Kind / Powder Technology 300 (2016) 2836 29
A lot of research contributions have been carried out regarding granules, as a function of the current state of the process. Particle
predicting the development of the PSD during granulation using popu- growth rates can be extracted from CFD for short process times (~ s).
lation balance equations (PBE) for small specic bed masses and low The development of PSD can nally be predicted for long process
spray ow rates. In order to solve PBE, it is necessary to know the in- times (~min) by transferring particle growth rates to PBE. The extended
ternal process variables, e.g. size-dependent growth rates or particle CFD-PBE model is applied to three different cases of a melt spray gran-
residence times in the spray zone, as a function of the current state ulation process in batch mode. The numerical results are validated
of the process. with experimental data.
Mrl [18] and Mrl et al. [19] dened three different equations to
obtain a particle growth rate for a granulation process considering 2. Methods and material
drop deposition. Thereby, the liquid ow rate of the nozzle is divided
into different fractions depending on the diameter, surface or volume 2.1. PBE model
of each particle phase. A lot of publications use the growth rate kinetics
of Mrl to model uidized bed sprays granulation processes [2023]. In the following we consider a batch-operated industrial melt spray
Hofmann et al. [24], Hampel et al. [25] and Meyer et al. [26] used a so- granulation process with negligible dust formation. For further informa-
called two-zone or multi-zone model to obtain the particle residence tion we refer to Section 2.3. For this case, the development of PSD can be
times of different particle sizes in a drying zone together with the particle described with a simple one-dimensional PBE as follows:
size-independent growth rate of Mrl in the spray zone. Hampel et al. val-
idated their population balance model for particle growth with a Wurster nGran GL dp nGran
0 1
granulator for small bed heights and low solution spray ow rates. There- t dp
fore, they used the residence times of Brner et al. [27], who investigated
the particle ow behavior in two-dimensional (2D) uidized bed granu- In order to solve this equation for a given initial condition, the
lation chambers. Brner et al. showed that the knowledge of residence knowledge of the size-dependent growth rate of the granules GL has
times of particles in the spray and drying zone of the granulation chamber to be known as a function of the current state of the process. Following
is very important to predict the particle growth in granulation processes. the work of Li et al. [28], the particle size-dependent growth rate can be
However, particle residence times depend on initial PSD, process param- obtained using a mass balance for each particle class i, considering the
eters and particle properties, and cannot be obtained by experiments for temporal deposited mass ow rate of droplets on particle class i:
three-dimensional industrial scale granulation processes.
Li et al. [28] developed a model using CFD and PBE to predict the de- dp;i 2 1 M_ m;i t
velopment of PSDs in continuously drying uidized bed spray systems GL;i dp;i ; t _ m;nozzle :
M 2
t 2 _
p Ni dp;i Mm;nozzle
with low solution spray ow rates (b5 kg/h) and small specic bed
masses (b 40 kg/m2). They validated their model with the experimental |{z}
K i t
results of Zank [9] and Grnewald [6].
The present work extends the model of Li et al. [28] to industrial
Hereby, M _ m;i t is the mass ow rate of melt droplets depositing
scale melt granulation processes with high spray ow rates (N 100 kg/h)
and high specic bed masses (N200 kg/m2) to predict the temporal on particle phase i. This unknown quantity can be obtained by a high
development of the product PSD and to optimize such type of processes temporal and spatial resolution of the granulation process using an
economically. advanced two-uid CFD multiphase model with ve uid phases. The
As will be shown in the following, with this model it is now possible model is solved for short process times (~s) considering uid dynamics,
to predict the temporal development of PSD during industrial scale particle growth due to drop deposition and energy equations. Extracting
granulation processes. For such predictions, it is necessary to evaluate M_ m;i t out of CFD and, subsequently, obtaining the time-averaged infor-
the internal process variables, e.g. size-dependent growth rates of the mation about GL(dp), the PBE can be nally solved to predict the
Fig. 1. Procedural method of the developed CFDPBE model. Growth rate kinetics are obtained by a high local and temporal CFD multiphase simulation and are used to solve population
balance equations for long process times. Numerical results are compared with a single-nozzle granulation experiment in batch mode.
30 P. Lau, M. Kind / Powder Technology 300 (2016) 2836
Table 1 interaction between particles and air for uidized beds can be described
Overview of computational multiphase models used for the ve-uid model. with the model of Gidaspow [11], who combined the models of Ergun
Euler phases 5 (air, 3 particle phases, melt) and Orning [31] and Wen and Yu [32]. In the case of the existence
Turbulence model k-Epsilon standard, dispersed of more than one particle phase, the interactions between particles
Timestep used 0.000010.0005 s are modeled with the symmetric model of Syamlal [33] and Syamlal
Solver Pressure-based, transient
et al. [34].
Gravity 9.81 m/s2
Drag particleair Gidaspow [11] The momentum exchange coefcients for granular ows include
Drag particleparticle Syamlal et al. [33] physical quantities which have to be modeled, for example, solids
Drag dropletair Schiller-Naumann [35] pressure, coefcient of restitution and radial distribution functions.
Granular viscosity Gidaspow [11]
Therefore, the so-called kinetic theory of granular ow is used.
Granular bulk viscosity Lun et al. [14]
Frictional viscosity Neglected
We refer to Gidaspow [11], Lun et al. [14], Syamlal et al. [33] and
Granular temperature Algebraic Syamlal et al. [34] for further information. An overview of general
Solids pressure Lun et al. [14] settings and multiphase model quantities used for the CFD simulation
Radial distribution Lun et al. [14] are specied in Table 1. These models were also used and validated
Packing limit 0.63; constant
with experiments by Li et al. [28].
Restitution coefcient 0.9; constant
Table 2
Different types of meshes for the grid independency study.
Table 3
Details of the geometry and boundary conditions.
A [mm] 1530
B [mm] 225
C [mm] 400
Geometry 2D rotationally symmetric
Number of nozzles 1
Boundary conditions Perforated Plate (B)
Nozzle
Wall (A)
Pressure outlet (C)
Symmetry axis
Droplet to nozzle tip ratio ddroplet
0:005
dnozzle
Air to liquid nozzle ratio _
M
ALR M_
air;nozzle
0:625
m;nozzle
v
Fluidization number f 2mm vperfPlate 1:8
mf ;2mm
_ m;nozzle t
M
Y t : 5
M_ Ref
Fig. 4. Measured and time-averaged normalized nozzle mass ow rate Y as a function of
time (Case 1).
Figs. 4, 5 and 6 show the ratio of mass ow rates of melt Y over time
for different cases. At the beginning, the melt mass ow rate of the noz-
zle is uctuating with very high amplitude due to the automatic regula-
tion of the nozzle. Due to the risk of crystallization of melt at the
beginning, the mass ow rate of the nozzle is low at the beginning to
avoid blocking and is increased stepwise until it reaches constant
mass ow rate. For the subsequent CFD-calculations these data were
time-averaged.
Fig. 7. Axial particle velocity in the cross-sectional area 100 mm above the perforated plate
Fig. 6. Measured and time-averaged normalized nozzle mass ow rate Y as a function of as a function of distance to the nozzle (x-coordinate) for three different meshes for a
time (Case 3). process time of 7 s.
P. Lau, M. Kind / Powder Technology 300 (2016) 2836 33
Fig. 8. Volume fraction of particle phase in the cross-sectional area 300 mm above the Fig. 10. Area-specic fraction of melt deposited Kias a function of time for three nodes
perforated plate as a function of distance to the nozzle (x-coordinate) for three different (Case 1).
meshes for a process time of 7 s.
M_ m;i t
X i t : 6
_ m;nozzle t
M
In the case that all melt droplets deposit on particle surfaces, the sum
of all Xi equals one:
X
N
X i X tot 1: 7
i1
Fig. 12. Area-specic fraction of melt deposited Kias a function of time for three nodes
Fig. 9. Drop deposition efciency for each node for the rst 25 s of the process (Case 1). (Case 3).
34 P. Lau, M. Kind / Powder Technology 300 (2016) 2836
It can be shown that the highest mass of droplets is deposited on 3.2. PBE simulation and experimental validation
node 2, which characterizes the particles with a diameter of 1.66 mm.
Due to the high mass fraction of the initial bed of this particle phase, a The particle growth rate has to be actualized for dened time inter-
high surface for drop deposition in the spray zone can be provided. It vals due to the unsteady behavior of the nozzle mass ow rate. There-
can be shown that the time-averaged total deposition efciency Xtot fore, the particle growth rate is implemented as a temporal stepwise
equals one, thus, the total mass of droplets entering the chamber is function which varies depending on the nozzle ow. It is assumed
deposited on the bed surface. This leads to the conclusion that there is that the drop deposition efciency fraction of each particle phase Xi is
no overspray, due to the high bed height. Experimental results also constant over time. Solving PBE for dened process times, we obtain
show that the effect of overspray can be neglected. Figs. 14, 15 and 16, which show the experimental (dots) and numerical
Due to the different surfaces of the nodes used in the simulation, Ki is results (lines) of the temporal development of the PSD q3(dp) in the
introduced, which normalizes the deposition efciency of melt Xi to the melt spray granulation process considering drop deposition for three
total surface of particle phase i (related to the total particle surface at the cases.
beginning, respectively). It can be assumed that the total area of each The experimental results show that the width of all PSDs increases
particle phase is constant for the rst few seconds of the process. with ongoing time. Large particles grow faster because of their higher
inertia and longer residence time in the spray zone compared to small
X i t particles. This correlation can also be described by the particle size-
K i t 8 dependent growth rate obtained. The experimental results can be predict-
Ai
ed quite well with the high-resolution CFD multiphase model followed by
solving PBE.
The area-specic fraction of melt deposited Ki is given in Figs. 10, 11
and 12 for the three cases, neglecting the rst 5 s of the unsteady
starting process of the nozzle ow. Ki has to be on the same level for
each node for a growth rate which depends only on the particle surface
fractions of particle phases. Obviously, Ki still seems to be a function of
residence time in the spray zone. Larger particles have a higher inertia,
therefore, the relative velocity between droplets increases with the in-
crease of particle diameter. This implies that larger particles can collect
more droplets during ight, related to their surface.
Due to the unsteady behavior of the uid dynamics of particles, Ki
has to be averaged in time to obtain a mean particle growth rate. There-
fore, the evolution of Ki is averaged for 20 s (neglecting the rst 5 s of
unsteady starting process) with a linear function. It can be shown that
the gradient of this function is near zero, so K i (time averagedKi) is
the y axis intercept.
Fig. 13. Particle size-dependent growth rate for three nodes (dots) for three different cases
(for the rst 25 s). A rst order approximation is carried out here (lines) to obtain a general Fig. 15. Comparison of numerical (CFD + PBE) and experimental results of the description
formulation of particle growth rate. of the temporal development of PSD (Case 2).
P. Lau, M. Kind / Powder Technology 300 (2016) 2836 35
The aim of this work was to extend the CFD-PBE model of Li et al. References
[28] and to apply it to a batch operated industrial uidized bed melt
spray granulation processes with high spray ow rates (N 100 kg/h) [1] L.-S. Fan, C. Zhu, Principles of Gas Solid Flows, Cambridge Univ. Press, Cambridge
[u.a.], 1998.
and a high bed mass (N 20 kg). Using this model, it is possible to predict [2] D. Geldart, Gas Fluidization Technology, Wiley, Chichester, New York, 1986.
the development of the PSD in melt granulation processes and to opti- [3] R. Jackson, The Dynamics of Fluidized Particles, Cambridge Univ. Press, Cambridge,
mize such type of processes economically. 2000.
[4] E.-U. Schlnder, E. Tsotsas, Wrmebertragung in Festbetten, durchmischten
Therefore, a 2D rotationally symmetric CFD advanced two-uid
Schttgtern und Wirbelschichten, Thieme, Stuttgart u.a, 1988.
model with ve uid phases model with one nozzle at its center was de- [5] S. Heinrich, L. Mrl, Fluidized bed spray granulationa new model for the descrip-
veloped. The ve uid phases were air, three particle phases and melt tion of particle wetting and of temperature and concentration distribution, Chem.
Eng. Process. 38 (1999) 635663.
(droplets). The model is solved for short process times (~s) considering
[6] G. Grnewald, Staubeinbindung und Keimbildung bei der Wirbelschicht-
uid dynamics, drop deposition (implemented with user-dened func- Sprhgranulation: Vom Prozessverstndnis zur Modellierung, Karlsruher Inst. fr
tions) and energy equations. The population balance was solved to pre- Technologie, Karlsruhe, 2010 (Diss.). (https://cuvillier.de/de/shop/publications/375).
dict the PSD for long process times (~min) by extracting size-dependent [7] M. Peglow, J. Kumar, G. Warnecke, S. Heinrich, L. Mrl, A new technique to deter-
mine rate constants for growth and agglomeration with size- and time-dependent
and time- and space-averaged particle growth rates from CFD, which nuclei formation, Chem. Eng. Sci. 61 (2006) 282292.
are not experimentally available. [8] S. Schaafsma, P. Vonk, N. Kossen, Fluid bed agglomeration with a narrow droplet
Comparison of numerical and experimental results shows that this size distribution, Int. J. Pharm. 193 (2000) 175187.
[9] J. Zank, Tropfenabscheidung und Granulatwachstum bei der Wirbelschicht-
method can predict the particle growth for a specic melt granulation Sprhgranulation, Univ., Diss. Karlsruhe, Shaker, Aachen, 2003.
case in batch mode quite well. Smaller deviations occur which can be [10] H. Uhlemann, L. Mrl, Wirbelschicht-Sprhgranulation: Mit 28 Tabellen, Springer,
minimized using more nodes for CFD simulation and with actualizing Berlin, 2000.
[11] D. Gidaspow, Multiphase Flow and Fluidization: Continuum and Kinetic Theory
Ki more often. As a future perspective, the CFD model will be validated Descriptions, Academic Press, Boston, 1994.
with other case studies. This model can also be extended to a continuous [12] J. Ding, D. Gidaspow, A bubbling uidization model using kinetic theory of granular
multi-stage granulation process for longer process times by updating ow, AICHE J. 36 (1990) 523538.
[13] J.T. Jenkins, S.B. Savage, A theory for the rapid ow of identical, smooth, nearly
particle size-dependent growth rates in time.
elastic, spherical particles, J. Fluid Mech. 130 (1983) 187.
[14] C.K.K. Lun, S.B. Savage, D.J. Jeffrey, N. Chepurniy, Kinetic theories for granular ow:
Nomenclature inelastic particles in Couette ow and slightly inelastic particles in a general
oweld, J. Fluid Mech. 140 (1984) 223.
ALR Air to liquid nozzle ratio, [].
[15] P.A. Cundall, O.D.L. Strack, A discrete numerical model for granular assemblies,
Ai Surface of particle phase i, [m2]. Gotechnique 29 (1979) 4765.
g Volume fraction of gas phase, []. [16] L. Fries, S. Antonyuk, S. Heinrich, S. Palzer, DEMCFD modeling of a uidized bed
p,i Volume fraction of particle phase i, []. spray granulator, Chem. Eng. Sci. 66 (2011) 23402355.
[17] M. Heine, S. Antonyuk, L. Fries, G. Niederreiter, S. Heinrich, S. Palzer, Modeling of the
i Volume fraction of Eulerian phase i, []. spray zone for particle wetting in a uidized bed, Chem. Ing. Tech. 85 (2013)
ddroplet Diameter of droplets, [m]. 280289.
36 P. Lau, M. Kind / Powder Technology 300 (2016) 2836
[18] L. Mrl, Anwendungsmglichkeiten und Berechnung von [28] Z. Li, M. Kind, G. Gruenewald, Modeling the growth kinetics of uidized-bed spray
Wirbelschichtgranulationstrocknungsanlagen, Techn. Hochsch., Magdeburg, granulation, Chem. Eng. Technol. 34 (2011) 10671075.
1980 (Diss.). [29] R.J. LeVeque, Finite Volume Methods for Hyperbolic Problems, Cambridge University
[19] L. Mrl, S. Heinrich, M. Peglow, Fluidized bed spray granulation, Handbook of pow- Press, Cambridge, New York, 2002.
der technology, vol. 12, Elsevier, Amsterdam [u.a.] 2007, pp. 21188. [30] R. Gunawan, I. Fusman, R.D. Braatz, High resolution algorithms for multidimensional
[20] S. Heinrich, M. Peglow, M. Ihlow, L. Mrl, Particle population modeling in uidized population balance equations, AICHE J. 50 (2004) 27382749.
bed-spray granulation analysis of the steady state and unsteady behavior, Powder [31] S. Ergun, A.A. Orning, Fluid ow through randomly packed columns and uidized
Technol. 130 (2003) 154161. beds, Ind. Eng. Chem. 41 (1949) 11791184.
[21] J. Drechsler, M. Peglow, S. Heinrich, M. Ihlow, L. Mrl, Investigating the dynamic be- [32] C.Y. Wen, Y.H. Yu, Mechanics of uidization, Chem. Eng. Prog. Symp. Ser. (1966)
haviour of uidized bed spray granulation processes applying numerical simulation 100111.
tools, Chem. Eng. Sci. 60 (2005) 38173833. [33] M. Syamlal, W. Rogers, T.J. O'Brien, MFIX Documentation, Theory Guide, vol. 1, National
[22] M. Dosta, S. Heinrich, J. Werther, Fluidized bed spray granulation: analysis of the Technical Information Service, Springeld, VA, 1993.
system behaviour by means of dynamic owsheet simulation, Powder Technol. [34] M. Syamlal, The Particleparticle Drag Term in a Multiparticle Model of Fluidization,
204 (2010) 7182. National Technical Information Service, Springeld, VA, 1987.
[23] A. Bck, S. Palis, E. Tsotsas, Model-based control of particle properties in uidised [35] F. Lfer, Staubabscheiden, Georg Thieme Verlag, Stuttgart, Germany, 1988.
bed spray granulation, Powder Technol. 270 (2015) 575583. [36] C.X. Bai, H. Rusche, A.D. Gosman, Modeling of gasoline spray impingement, Atomi-
[24] T. Hoffmann, M. Peglow, E. Tsotsas, Prozessdynamik der Wirbelschichtgranulierung, zation Sprays 12 (2002) 128.
Chem. Ing. Tech. 83 (2011) 658664. [37] M.R.O. Panao, A.L.N. Moreira, Experimental study of the ow regimes resulting from
[25] N. Hampel, A. Bck, M. Peglow, E. Tsotsas, Continuous pellet coating in a wurster u- the impact of an intermittent gasoline spray, Exp. Fluids 37 (2004) 834855.
idized bed process, Chem. Eng. Sci. 86 (2013) 8798. [38] Z. Li, Fortgeschrittene Methoden zur Beschreibung der Wirbelschicht-
[26] K. Meyer, A. Bck, E. Tsotsas, Dynamic multi-zone population balance model of par- Sprhgranulation(KIT, Diss.) Karlsruher Institut fr Technologie, Karlsruhe, Baden,
ticle formulation in uidized beds, Procedia Eng. 102 (2015) 14561465. 2013 (KIT Scientic Publishing).
[27] M. Brner, M. Peglow, E. Tsotsas, Particle residence times in uidized bed granula- [39] R.G. Gordon, Error bounds in spectroscopy and nonequilibrium statistical mechanics,
tion equipments, Chem. Eng. Technol. 34 (2011) 11161122. J. Math. Phys. 9 (1968) 1087.