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Accepted Manuscript

Title: Counter-current spray drying with stream separation:


Computational modeling of a novel dryer design

Author: Soheil Soltani Per Gerde Fernando Acevedo Anders


Rasmuson

PII: S0263-8762(14)00252-4
DOI: http://dx.doi.org/doi:10.1016/j.cherd.2014.05.023
Reference: CHERD 1601

To appear in:

Received date: 4-10-2013


Revised date: 16-4-2014
Accepted date: 19-5-2014

Please cite this article as: Soltani, S., Gerde, P., Acevedo, F., Rasmuson,
A.,Counter-current spray drying with stream separation: Computational modeling
of a novel dryer design, Chemical Engineering Research and Design (2014),
http://dx.doi.org/10.1016/j.cherd.2014.05.023

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Highlights

 Novel spray dryer design

 Fine powder for inhalation

 CFD model

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Page 1 of 34
Counter-current spray drying with stream separation: Computational
modeling of a novel dryer design
Soheil Soltani a, Per Gerde b, Fernando Acevedo b, Anders Rasmuson a, *
a
Chemical and Biological Engineering, Chalmers University of Technology, SE-412 96 Göteborg, Sweden

b
Inhalation Sciences Sweden AB, SE-171 77 Stockholm, Sweden

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Abstract

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Spray drying has been in use for producing fine powder of pharmaceuticals in order to make
the drug respirable and thus accessible to the large absorptive area of the lungs. However,

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traditional designs for spray dryers have turned out to be inappropriate for processing very
fine particles. Therefore, a novel design has been suggested in which the drying agent is
separated from the moisture-containing material by using a vapor-permeable membrane

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(Gerde, 2009). A computational model of the new design has been developed for design and
optimization purposes. The model has been shown to satisfactorily reproduce the
experimental measurements. A linear correlation has been obtained between the swirl flow
rate and the outflow concentrations, predicting a maximum possible flow rate of 1 L/min in
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order to meet the required quality of the product. The performance of the dryer has been
shown to be very sensitive to the injection flow rate as well as the effective diffusivity of the
membrane. Using ethanol as the solvent, the model predicts a maximum injection of 12
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mg/min. Based on the simulation results, a fairly low probability of wall deposition is
expected.
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Keywords: Spray drying; Membrane; Computational modeling; Nebulizer


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1. Introduction
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Spray drying is a popular unit operation for processing dry powder of solid material. It has
particularly been used in pharmaceutical and food industry, mostly because of the fact that the
residence time of the solid material inside the dryer is short, and this is an important
advantage in the case of temperature-sensitive materials. Furthermore, the state of the final
product, that is a solid powder, is the desired one in the aforementioned industrial
applications. A novel design for a spray dryer has been introduced by Gerde et al. (Gerde,
2009; Gerde et al., 2010), which has been shown to be able to produce a very fine powder
suitable for pharmaceutical applications. In addition to that, the main advantage of this novel

*
Corresponding author. Address: Department of Chemical and Biological Engineering, Chalmers University of
Technology, SE-412 96 Göteborg, Sweden.
Telephone: +46 31 772 29 40
Email address: rasmuson@chalmers.se

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Page 2 of 34
configuration is that a large amount of solvent is diffused through the membrane and thus
removed from the drying chamber before the product is collected on a filter downstream the
drying column. Therefore, the probability of agglomeration in the final product is
substantially reduced, and a very fine and dry powder is obtained at a high yield. Using the
filter for collecting the product reduces the losses and makes the equipment convenient for
handling the powder of precious material in small scales (Gerde et al., 2010). In the present
paper, characteristics of the new design are investigated by developing a computational model

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for the equipment.

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Traditional models for spray drying treat the dryer as a ‘black box ‘and consequently very few
details of the important phenomena taking place inside the dryer are obtained. Such models

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are not able to predict the occurrence of wall deposition, particle size distribution (PSD) and
agglomeration between the particles, and they can hardly be used for up scaling applications

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(Blei and Sommerfeld, 2007). Various modeling approaches with different degree of
complexity from the traditional to the more rigorous ones have been reviewed in the literature
(Langrish, 2009). One approach, which is also known as the coarsest-scale, is to describe the
drying column as a combination of well-mixed, plug flow and bypass zones and to write the

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overall balance equations accordingly. Considering the height-to-diameter ratio of the drying
column, an aspect ratio of larger than 5 corresponds to a tall-form design. The flow pattern in
many regions is then expected to be close to plug flow. On the other hand, short form
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columns have a broader residence time distribution and exhibit a well-mixed behavior.

A finer scale representation can be developed in which a parallel flow is assumed between the
gas and particulate phases. This approach is more suitable for tall form dryers and has been
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used by Truong et al., assuming a uniform distribution of the gas phase velocity in the radial
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direction with the radial and tangential velocity components being negligible (Truong et al.,
2005). However, this assumption neglects the effect of swirl flow and the possible
recirculating regions that are common in the conical designs of a drying chamber. Information
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about the drying rate of the particles is then used to calculate the heat and mass transfer
to/from the particles as well as the gradual changes in particle diameter.
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A more rigorous manner of dealing with the gas phase velocity profile has been examined by
Zbicinski, in which the velocity components are calculated using computational fluid
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dynamics (CFD), and thus the complete information of the velocity field is obtained
(Zbicinski, 1995).

The level of accuracy and thus complexity of the model can be increased by accounting for
the coupling effects between momentum, heat and mass transfer, which forms the foundations
of the Particle Source in Cell method (PSI-Cell) (Crowe et al., 1977). These coupling effects
give rise to the profiles of concentration, temperature, velocity and pressure within the
continuous phase. Furthermore, the knowledge of the particle trajectories directly determines
the amount of time each particle spends inside the chamber, which is of great importance in
the case of temperature sensitive material (Gauvin et al., 1975). This framework has therefore
been used as the modeling approach in the present study.

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The importance of the flow field pattern and its influence on the performance of spray dryers
have been pointed out previously (Langrish and Fletcher, 2001). Due to complexities in the
geometry, numerical techniques are required in order to solve the Navier-Stokes equations.

The aim of this work is to develop a computational model for evaluating the novel design of a
spray dryer. The model has been used for investigating the effect of various design parameters
such as swirl flow rate, membrane diffusivity and injection rate on the performance of the

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dryer.

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2. The spray dryer system

The dryer consists of an 85-cm long annular column, as shown in Figure 1. The interior

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column is 49 mm in its inner diameter and is made of a perforated, steel tube with 53% void
area, as shown in Figure 2. The external surface of the inner column is covered with a vapor-
permeable membrane, which is a thin layer of rice paper with ~10-14 g/m2 specific weight
and a measured thickness of around 50 µm. The external column consists of a steel tube with

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an inner diameter of 9.5 cm, in which a stream of moisture-free air flows counter-currently on
the exterior side of the membrane at a flow rate of 30-50 L/min, sweeping out the diffused
moisture. In order to facilitate both the motion of the droplets and mass transfer towards the
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membrane, a swirling air stream of 1 L/min flows inside the inner column. As depicted in
Figure 3, a gas diffuser with an inner diameter of 5 cm has been used for this purpose, which
consists of 40 equidistant holes. Each hole has a diameter of 1.5 mm and is made at an angle
of 20o with respect to the normal direction to provide a gently rotating air flow which has a
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tangential and a radial component. The direction of the latter is towards the centerline of the
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inner column and therefore helps preventing wall deposition of the generated aerosol. In order
to further prevent wall deposition, the swirl flow rate is chosen so that the flow regime
remains laminar inside the drying column. Thus the air streams are separated, but the
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membrane allows for the diffusion of the vapor phase through. Although the equipment is
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small compared to the industrial dryers, its capacity is justified by the product’s value.

The injection system utilizes the Aeroneb Pro mesh nebulizer, which works based on the
action of a piezoelectric actuator (Aerogen, 2011). The nominal flow rate of the nebulizer is
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reported as 0.4 mL/min, but the dryer normally works at less than 5% of this value. The
piezoelectric device works at a constant frequency, and consequently the injection flow rate is
also fixed. However, it is possible to use a control scheme to periodically turn the electric
current on and off, so that a pause is introduced in between the injections. The duration of the
pause then determines the net flow rate over a certain period. The spray-dried product is
finally collected on a filter, which is situated at the bottom of the interior column.

Figure 1. Schematic representation of the spray dryer. The figure has been scaled by a factor of 0.5 in the axial
direction for the sake of visualization.

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Figure 2. Perforated tube.

Figure 3. The top lid of the dryer. The perforated gas diffuser surrounding the plastic mouth of the nebulizer
provides the swirl flow.

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3. Experimental

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Using pure ethanol as a common solvent in pharmaceutical applications, the performance of
the dryer has been examined by steady state measurements of the solvent concentration in the

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outflows. The result has been particularly useful for validating the model’s prediction of the
cut-off in the solvent concentrations between the interior and exterior regions of the column.

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The information about the operating conditions of the dryer for the three experimental cases is
included in Table 1. The inflow streams enter the dryer at 293 K. In a different experiment, a
10% w/w solution of lactose in water was spray dried in order to investigate wall deposition
and the extent of agglomeration between the particles. The solution is injected into the interior

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column in the form of micronized droplets with an average diameter of around 4 µm (Gerde,
2009; Gerde et al., 2010).
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The spray dried product has been characterized by Scanning Electron Microscopy (SEM);
furthermore, the powder was re-aerosolized using dustgun aerosol technology (Gerde et al.,
2004), and the generated aerosol was sized on a Marple cascade impactor to obtain the
particle size distribution (PSD) (Rubow et al., 1987).
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4. Modeling approach
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4.1 Discrete particle method


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The Eulerian-Lagrangian framework has been used to model the dispersed, two-phase flow
inside the dryer. The continuous phase is treated as Eulerian, and the Navier-Stokes equations
along with the transport equations of heat and species’ concentrations have been solved
numerically using Computational Fluid Dynamics (CFD). The discrete particles are
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represented in the Lagrangian context, in which the equation of motion is written for the
particles using Newton’s second law (Crowe, 2012).

An important issue is the degree of coupling in the two-phase system of particles and gas.
Stokes number (St) is defined as the ratio between the particle relaxation time and the time
scale of the changes in the flow field:

p
St  (1)
f

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Therefore, for St<<1 the phases can be considered to be one-way coupled. In this case,
particles follow the flow completely, while the continuous phase does not sense the presence
of the particles. The particle relaxation time is calculated from:

 pd p2
p  (2)
18 f

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which takes a value of 6  10 5 ( s) in the current case. The time scale of the flow field is not

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known a priori, but since the prevailing regime is laminar, the time scale of the changes in the
flow field is expected to be some orders of magnitude larger than the time required for the

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dispersed phase to respond to those changes. Consequently, the order of magnitude estimation
indicates St<<1 and this is intuitively justified considering the very small size of the particles.

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Another important parameter that should also be considered in order to determine the degree
of hydrodynamic coupling is the volume fraction of the dispersed phase,  d , which is defined
as

V V
 V 
 d  lim  d 
 V 
0

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where V0 is the size of the averaging volume which guaranties smooth variation of the
averaged property and must be much larger than the particle volume while being much
smaller than the physical dimensions of the system. Therefore, a computational cell can be
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used for calculating  d . The highest volume of the dispersed phase (Vd ) can be encountered
in the first computational cells adjacent to the injection point where droplets have not yet
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completely dispersed. For such an extreme case,  d is calculated to be around 0.1%, and
consequently it can be concluded that the phases are hydrodynamically one-way coupled. The
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fairly low value of  d implies that the mutual interactions between the particles can be
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neglected.

Heat and mass transfer, however, are two-way coupled between the two phases due to the
profiles of concentration and temperature induced by the evaporation from the droplets.
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4.2 Droplet evaporation

To be able to compare the simulation results with the experimental data, the discrete phase is
assumed to consist of pure ethanol with no dissolved material. This assumption also reduces
the computational cost, since internal mass and heat transfer resistances can be neglected.
Convective transport of the moisture that originates from the droplet evaporation can be
correlated to the mass transfer coefficient, assuming a uniform distribution of the fluid density
and velocity over the surface of the droplet (Crowe, 1980):

dm
 kcd p2 ( X   X s ) (4)
dt

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where X s , X  represent the mass fraction of the moisture at the droplet surface and in the
bulk, respectively. X s can be calculated assuming saturation conditions on the surface of the
droplet, and k c , d p are mass transfer coefficient and particle diameter, respectively. The mass
transfer coefficient can be obtained from the Sherwood number, Sh , which in spray drying is
often calculated using the Ranz-Marshall empirical correlation:

Sh  D

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kc  (5)

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dp

Sh  2  0.6 Re1 / 2 Sc1 / 3 (6)

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Sc is the Schmidt number, which is dependent on the composition of the carrier phase, and D
is the mass diffusivity.

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Similar to the mass transfer calculation in each iteration, heat transfer to the droplet is
calculated in an analogous way to update the droplet’s temperature:

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.
Q  hd p2 (T  T p ) (7)

with h being the heat transfer coefficient of the carrier phase. T and Tp are the temperatures of
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the carrier phase and the droplet, respectively. The heat transfer coefficient is obtained from the
Nusselt number which is in turn calculated from the Ranz-Marshall correlation:
d

Nu  k
h (8)
dp
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Nu  2  0.6 Re1 / 2 Pr1 / 3 (9)


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dT p . dm p
m pC p  Q  (10)
ce

dt dt

Pr and k are the Prandtl number and the thermal conductivity of the carrier phase,
respectively. Radiative heat transfer is neglected and Cp and  represent the droplet heat
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capacity and latent heat of evaporation, respectively. Since the evaporation takes place under
atmospheric pressure and at the wet-bulb temperature, a constant latent heat of evaporation
was assumed for the liquid droplets.

4.3 Mass transfer through the porous membrane

Considering the high flow resistance of the membrane and the negligible pressure difference
between the interior and exterior columns, any bulk flow through the membrane, i.e. normal
to the main flow direction, can be neglected. Therefore, molecular diffusion is the only
important mechanism of transport through the membrane, and due to the rather large pore size
of the membrane, the diffusion mechanism can be assumed to be ordinary diffusion, i.e. the
Knudsen mechanism is neglected (Welty et al., 2007). In the CFD model, the membrane has

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been treated as a porous zone with a very large viscous resistance which restricts the flow,
and diffusion through the membrane is quantified by providing the solver with an effective
diffusivity for ethanol. Due to the fairly low thermal mass of the thin membrane, it is assumed
to be in thermal equilibrium with the surrounding gas. This assumption substantially increases
the stability and reduces the computational cost of the model.

Effective diffusivity of the membrane is dependent upon its porosity and tortuosity denoted
by  and  , respectively (Ma et al., 2014; Nilsson and Stenstrom, 1995):

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Deff  D (11)
2

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The porosity of the membrane is calculated to be ~0.84 considering an average specific
weight of ~12 g/m2 for the rice paper and its measured thickness (c.f. section 2). An

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assumption is made in the calculation of the porosity that the paper is almost entirely made up
of alpha-cellulose, having a density of ~1500 kg/m3.

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However, the tortuosity factor is not straightforward to obtain rigorously due to its inherent
stochastic properties originating from the random orientation of the pores. We have chosen
two methods from the literature; one based on an empirical correlation for tortuosity and the
other being Lord Rayleigh’s analysis of heat and mass transport in porous media. The
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following empirical correlation between the porosity and tortuosity of porous media has been
chosen to estimate the effective diffusivity of the membrane assuming the pores to be
represented by the flow channels formed in a packed-bed of spherical particles (Comiti and
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Renaud, 1989; Tang et al., 2012; Wyllie and Gregory, 1955):


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1
  1  0.41ln( ) (12)

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The result is then compared with the model proposed by Lord Rayleigh, which derives a
correlation between the porosity and thermal conductivity of porous media assuming the
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medium to be composed of cylindrical pores oriented in rectangular order. Using the analogy
between the differential equations describing heat and mass transport in porous media, the
following relationship between the gas phase diffusivity and the effective diffusivity of the
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membrane is established (Nilsson and Stenstrom, 1995; Rayleigh, 1892):


Deff ~ D (13)
2 

Consequently, a tortuosity factor of ~1.07 is calculated using the empirical correlation as


mentioned above, which predicts: Deff  0.73D . This is in close agreement with the
prediction of the Lord Rayleigh’s model which estimates the effective diffusivity to be
0.72 D . The effective diffusivity of the membrane is therefore considered to be
Deff ~ 8.34 106 m2/s (the molecular diffusivity of ethanol in air at room temperature is

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D ~ 11.5 10 6 m2/s). The result is then incorporated in the numerical solver through a user’s
defined function (UDF).

4.4 Computational model

A three-dimensional model that accounts for a 30o periodic segment of the overall system has
been put up and discretized into 95000 cells. The average cell size is 1.13 108 m3 and the
cells have a minimum orthogonal quality of 0.16. The membrane has been treated as a porous

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zone, and the drag law for a sphere according to Morsi and Alexander has been used to
calculate the drag force on the discrete particles (Morsi and Alexander, 1972):

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a2 a
C D  a1   32 (14)
Re Re

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where C D is the drag coefficient and a1 , a2 and a3 are the constants given over a range of
Reynolds numbers. The momentum equation was discretized by using the 2nd order, upwind
scheme, while the transport equations of energy and the species’ concentrations were

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discretized using the third order, MUSCL scheme (ANSYS® Academic Research, 2011).

A steady state solution of the continuous phase is then obtained by solving the discretized
equations with a multigrid solver. The discrete phase is treated in an unsteady fashion, with a
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particle time-step size of 0.01 s, which implies stepwise particle tracking while accounting for
the coupling between the two phases. Time-marching of the equation of motion was
controlled by choosing a time-step of 3 10 5 ( s) to be smaller than the particle relaxation
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time (c.f. section 4.1). Despite ensuring an accurate tracking scheme, such a fine time-
resolution substantially increases the computational time of the model to a few days on a 4-
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core CPU with 3.40 GHz clock frequency and 16 GB memory.


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4.4.1 Boundary conditions

A uniform velocity profile, normal to the boundary is assumed at the drying air inflow. The
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angle at which the swirling flow leaves the gas diffuser has been used to decompose the
velocity vector in cylindrical coordinates. Thus the projection of a unitary vector into radial
and tangential coordinates gives the components of the velocity vector as 0.94 | v | and
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0.34 | v | , respectively. All the inflow streams enter the column at room temperature, and
natural convection with the surroundings is assumed at the external wall of the dryer. The
discrete phase trajectory is terminated upon collision with the physical boundaries.

4.4.2 Simulation quality

Convergence criteria for the flow field variables as well as species’ concentrations were
satisfied by obtaining absolute residuals of smaller than 110 5 . Solution to the energy
equation was converged if a residual of smaller than 1  10 8 was met. A grid-independent
solution has been obtained by comparing the simulation results with those obtained on a finer
mesh. The grid was locally refined down to an average cell size of 4.7  10 9 m3 in regions

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with significant gradients (e.g. in the vicinity of the membrane); consequently the absolute
mass imbalance of the converged solution was reduced to less than 9  10 15 kg/s.

5. Results and discussion

The basis for the simulation results is the second experimental case, as shown in Table 1,

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section 3.

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5.1 Flow field

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A laminar flow field is established in the inner region with the Reynolds number in the range
of 155-160. In order to investigate the probability of wall deposition, simulation results of the
radial velocity have been analyzed. Figure 4 shows the resulting profile along the drying

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column, obtained at a radial distance of 2 cm from the centerline, i.e. fairly close to the
interior wall where the presence of a radial flow is most crucial.

Figure 4. Radial velocity along the column (case 2).

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The radial component of the swirl flow damps out after ~7 cm from the top of the column,
indicating a rather low probability of wall deposition in the initial part of the drying column.
This is further strengthened by studying the SEM image of the spray-dried lactose, as shown
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in Figure 5, which also indicates a rather uniform and intact product. The measured
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aerodynamic diameter of spray dried lactose is shown in Figure 6, indicating that the final
product varies in median diameter from 2 to 5 µm. However, wall deposition may be expected
to some extent in the region close to the injection port with an effectively negligible swirl
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flow in the radial direction.


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Figure 5. SEM image of spray-dried lactose.


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Figure 6. Measurements of the aerodynamic diameter of spray-dried lactose (Gerde et al., 2004; Rubow et al.,
1987)

5.2 Temperature distribution

A contour plot of temperature distribution is shown in Figure 7. Droplet evaporation at the


core of the spray is almost entirely due to heat transfer from the air. This corresponds to the
wet-bulb temperature of the mixture, which is ~275 K for air-ethanol, as predicted by the
simulation results.

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Figure 7. Temperature distribution.

5.3 Concentration distribution

A comparison has been made between the simulation results and the experimental

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measurements of the solvent concentrations at the outflows of the dryer. The results are

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shown in Table 2, indicating a reasonably good performance of the model. The concentration
distribution throughout the dryer is shown in Figure 8.

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Figure 8. Concentration distribution inside the dryer.

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5.4 Particle trajectories

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The aerosol cloud consists of micron-sized droplets, which evaporate so rapidly that their
trajectories terminate within less than 10 cm from the top of the drying column. The residence
time of the particles is in the range of 0.01-0.32 s, and the particles’ Reynolds number varies
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between 110 7 and 110 4 . A plot of particle size vs. the axial position of the particles is
illustrated in Figure 9a.
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Figure 9. a) Particle size as a function of particles’ axial position relative to the top of the column. b)
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Streamlines of the flow field at the top of the drying column.


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In a more realistic case where solid particles are formed during the course of drying, the
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trajectories will span the entire drying column. Nevertheless, the assumption of one-way
coupling between the two phases will still be valid, since the particle relaxation time from Eq.
(2) will be less than 2 10 4 ( s) (assuming lactose as the solid phase, having a density of
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~1520 kg/m3). Therefore, it is expected that the particles will still follow the streamlines of
the flow field completely. Such streamlines are calculated and shown in Figure 9b. For the
sake of visualization, only the top part of the column where the swirl flow dominates is
depicted; the streamlines in the rest of the column have the typical shape of a laminar flow
field in a duct. It is important to note that the streamlines of the rotating flow are mainly in the
center of the column, indicating that the probability of the particles being drifted towards the
wall because of this rotating flow is negligible.

5.5 Design parameters

The effect of various flow rates and effective diffusivities of the membrane on the
performance of the dryer has been studied using the CFD model.

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5.5.1 Swirl flow rate

The existence of a swirling flow inside a drying chamber is known to be generally helpful for
flow stability, especially in the presence of a strong jet flow of the spray. This is mainly
because of increasing the spray width and thereby allowing the pressure field downstream of
the dryer to counteract the axial momentum of the jet. By increasing the strength of the swirl
flow, the recirculating zone eventually becomes unstable, resulting in a breakdown and the

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precession of the vortex. In this regime, the flow pattern is strongly unsteady, and

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consequently an increase in wall-deposition is a potential concern. Prolonged residence-time
of the particles that are trapped in the recirculating zones is the other adverse effect of swirl
flows in spray drying of temperature-sensitive material. Nevertheless, a swirling flow

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enhances the mixing between the aerosol and the gas phase and is required for efficient
spreading of the aerosol puff (Southwell and Langrish, 2001).

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In the current design, the injected aerosol has a quite low axial momentum, and there is no
spray jet as such. Therefore, the swirl inflow has been designed to produce a gently rotating
flow whose axis of rotation coincides with the main axis of the annulus. In this way, the

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rotating flow helps stabilizing the injected aerosol and acts as a carrier phase, providing the
discrete phase with the required momentum to pass through the dryer. Consequently, vortex
precession, wall-deposition and the aforementioned recirculating zones are avoided, while
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efficient spray-air mixing and spreading of the aerosol cloud are achieved, which also makes
it possible to treat the flow field as steady state (c.f. section 4.4).

As the carrier phase, the swirl flow rate affects the concentration distribution in the dryer,
d

since it determines the residence time distribution of the particles and the evaporated moisture
in the interior column. Further investigation reveals that at constant injection and drying air
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flow rate solvent concentration increases linearly with the swirl flow rate in the outlet of the
drying column. In contrast, increasing the swirl flow rate causes the solvent concentration to
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decrease in the outlet of the exterior column. The results obtained from the model are shown
in Figure 10 for the injection flow rate of 1.62  10 7 kg/s and the drying air flow rate of
ce

41.17 L/min. Regression analysis shows a linear dependence of both outflow concentrations
on the swirl flow rate:

Ci  8.35  106 q  3.1  10 6 ; R 2 adj.  0.9985


Ac

Ce  3.21  10 7 q  5.46  10 6 ; R 2 adj .  0.9898

where Ci and Ce are outflow concentrations of ethanol corresponding to interior and exterior
column, respectively, and q is the swirl flow rate.

Practical experience suggests that in order to prevent the risk of agglomeration in the final
product, solvent retention in the drying column outflow should be kept below 2% (mol/mol).
For constant injection and drying air flow rates, as mentioned above, the percentage of solvent
retention as a function of the swirl flow rate has been calculated as shown in Figure 11.

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Page 12 of 34
Regression analysis of the results shows a power relation between solvent retention and the
swirl flow rate:

SR  0.03q 3.46 ; R 2 adj.  0.999

where SR and q are the percentage of solvent retention and swirl flow rate, respectively. It can
be predicted that under the specified injection and drying air flow rates, the maximum
possible swirl flow rate should be around 0.89 L/min.

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Figure 10. Simulation results of the impact of swirl flow rate on ethanol concentration at the outlet of the drying

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column (o) and of the exterior column (*)

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Figure 11. Percentage of solvent retention as a function of swirl flow rate

5.5.2 Injection flow rate


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The model has been used in order to predict the outflow concentrations for various injection
flow rates, and the results are shown in Figure 12. The swirl flow rate is 0.48 and the drying
air flow rate is 45.87 L/min, according to the second experimental case. As shown in Figure
d

12, the injection flow rate is strongly limited by the drying capacity of the column, which is
the major drawback of the equipment. A larger design becomes inevitable if the full capacity
te

of the nebulizer is desired to operate on, as significant solvent retention has been observed in
the product at above 1.5 107 kg/s injection rate.
p
ce

Figure 12. Simulation results of ethanol concentration at the exterior column outflow (*) and at the drying
column outflow (o) as a function of injection flow rate
Ac

5.5.3 Effective diffusivity of the membrane

The outflow concentrations of ethanol have been calculated for a number of different values
for the effective diffusivity of the membrane, and the results are shown in Figure 13a. The
percentage of solvent retention has also been calculated for each data point, as shown in
Figure 13b. The lowest possible diffusivity which still keeps the solvent retention below 2%
would be 2.55 10 6 m2/s. Simulation results in Figure 13a indicate two distinct regimes of
mass transfer through the membrane, namely a diffusion-controlled and a flow-regime. It is
observed that decreasing the effective diffusivity of the membrane from its estimated value
does not have any significant effect on the concentration of ethanol in the outflows initially,
which indicates that transport through the boundary layer in the gas-phase is the rate-

12
Page 13 of 34
determining step. A further decrease in the effective diffusivity results in sharp changes in the
concentration distribution, indicating a diffusion-controlled regime. It is stressed that the
flow-regime is the desired operating condition of the dryer in which the bulk flow through the
membrane is restricted but not vapor diffusion.

Figure 13. Simulation results of ethanol concentration at exterior column outflow (a,*), drying column outflow
(a,o), and the percentage of solvent retention (b) as a function of effective diffusivity of the membrane

t
ip
cr
6. Conclusions

The novel design for the spray drying of micron-sized particles has been studied, and a model

us
for the system has been obtained based on the Eulerian-Lagrangian approach. The model has
been shown to be able to reproduce the experimental data from the dryer and consequently
can be used for investigating the effects of various design parameters. The performance of the

an
dryer under various operating conditions has been studied by conducting a parameter study
based on the derived model. One limitation of the current design is its incapability of handling
the generated aerosol if the injection system runs at nominal capacity. This problem could be
remedied with a lower output nebulizer with fewer mesh pores that would allow a continuous
M
operation of the injection system. However, a major advantage of the current design is the
removal of a large amount of solvent so that the solvent concentration at the drying column
outflow can be significantly reduced.
d
p te
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Nomenclature

Constants of the drag law [-]

t
a

ip
kmol
C Concentration [ ]
m3

cr
CD Drag force coefficient [-]

us
J
Cp Heat capacity [ ]
kg.K

Diameter [ m ]

an
d

m2
D Molecular diffusivity [ ]
s
M
W
h Heat transfer coefficient [ ]
m2 K
d

W
k Thermal conductivity [ ]
m.K
te

m
kc Mass transfer coefficient [ ]
p

m Mass [kg]
ce

Nu Nusselt number [-]

Pr Prandtl number [-]


Ac

L
q Swirl flow rate [ ]
min
.
Q Heat transfer rate [W]

Re Reynolds number [-]

Sc Schmidt number [-]

Sh Sherwood number [-]

St Stokes number [-]

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SR Percentage of solvent retention [% mol/mol]

t Time [s]

T Temperature [K]

X Mass fraction [-]

V

t
Control volume for averaging [ m3 ]

ip
cr
Greek symbols

 Volume fraction [-]

us
 Porosity [-]

 Tortuosity [-]

an
λ Latent heat of evaporation [J/kg]

 Viscosity [Pa.s]
M
kg
 Density [ ]
m3
d

 Time scale [s]


te

Subscripts
p

d Dispersed phase
ce

e External column

eff Effective diffusivity


Ac

f Continuous phase

i Interior (drying) column

p Particulate phase

s Surface condition

w Wet-bulb temperature

 Bulk condition

15
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References

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t
ANSYS® Academic Research, 2011. ANSYS FLUENT Theory Guide, Release 14.0 ed. ANSYS Inc.,

ip
Canonsburg, PA.
Blei, S., Sommerfeld, M., 2007. CFD in Drying Technology – Spray-Dryer Simulation, Modern Drying

cr
Technology. Wiley-VCH Verlag GmbH & Co. KGaA, pp. 155-208.
Comiti, J., Renaud, M., 1989. A New Model for Determining Mean Structure Parameters of Fixed-
Beds from Pressure-Drop Measurements - Application to Beds Packed with Parallelepipedal Particles.

us
Chem Eng Sci 44, 1539-1545.
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an
Flows. Journal of Fluids Engineering-Transactions of the Asme 99, 325-332.
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M
TECHNOLOGIES AB (Fogdevreten 2B, S-SE - Stockholm, 171 77, SE),Gerde, Per (Römora Självfräten, S-
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Gerde, P., Ewing, P., Lastbom, L., Ryrfeldt, A., 2004. A novel method to aerosolize powder for short
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d

Inhalation Toxicology 16, 45-52.


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Fine Powders at Ambient Temperature in High Yields. Respiratory Drug Delivery 2, 605-608.
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p

Langrish, T.A.G., Fletcher, D.F., 2001. Spray drying of food ingredients and applications of CFD in
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ce

Ma, Q., Chen, Z.Q., Shi, J., Li, D., 2014. Lattice Boltzmann modeling of VOC desorption and diffusion in
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Ac

Nilsson, L., Stenstrom, S., 1995. Gas-Diffusion through Sheets of Fibrous Porous-Media. Chem Eng Sci
50, 361-371.
Rayleigh, L., 1892. LVI. On the influence of obstacles arranged in rectangular order upon the
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Tang, X.W., Sun, Z.F., Cheng, G.C., 2012. Simulation of the relationship between porosity and
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Truong, V., Bhandari, B.R., Howes, T., 2005. Optimization of co-current spray drying process of sugar-
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Welty, J., Wicks, C.E., Rorrer, G.L., Wilson, R.E., 2007. Fundamentals of Momentum, Heat and Mass
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t
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Table 1. Experimental cases

Parameters Experimental case


1 2 3

Injection flow rate, (kg/s) 1.62E-07 1.54E-07 1.62E-07


Drying air flow rate, (L/min) 41.13 45.87 41.17
Swirl flow rate, (L/min) 0.45 0.48 0.4

t
ip
Table 2. Model predictions vs. experimentally measured outflow concentration of ethanol.

cr
External column
Measured concentration Model prediction
Experimental case
[kmol/m3] [kmol/m3]

us
1 4.97 10 6 4.80  10 6
2 4.35  10 6 4.38 10 6
3 5.12  106 5.14 106

an
Drying column
Measured concentration Model prediction
Experimental case
[kmol/m3] [kmol/m3]
1 5.99 10 7 6.95 107
M
2 7.09  10 7 7.47  107
3 4.04  107 5.57 107
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2.17e-14 1.17e-04 2.33e-04 3.50e-04 4.67e-04 5.83e-04 7.00e-04 8.17e-04 9.34e-04 1.05e-03 1.17e-03
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