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Multi-Scale Multiphase Modeling of Transport Phenomena in Spray-Drying


Processes

Article  in  Drying Technology · January 2015


DOI: 10.1080/07373937.2014.941110

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Multi-Scale Multiphase Modeling of Transport


Phenomena in Spray-Drying Processes
a b b
Maksim Mezhericher , Avi Levy & Irene Borde
a
Center for Engineering Modeling, Design and Numerical Simulations, Department of
Mechanical Engineering , Shamoon College of Engineering , Beer-Sheva , Israel
b
Pearlstone Centre for Aeronautical Engineering Studies, Department of Mechanical
Engineering , Ben-Gurion University of the Negev , Beer-Sheva , Israel
Accepted author version posted online: 29 Jul 2014.Published online: 19 Nov 2014.

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To cite this article: Maksim Mezhericher , Avi Levy & Irene Borde (2015) Multi-Scale Multiphase Modeling of
Transport Phenomena in Spray-Drying Processes, Drying Technology: An International Journal, 33:1, 2-23, DOI:
10.1080/07373937.2014.941110

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Drying Technology, 33: 2–23, 2015
Copyright # 2015 Taylor & Francis Group, LLC
ISSN: 0737-3937 print=1532-2300 online
DOI: 10.1080/07373937.2014.941110

Review Article
Multi-Scale Multiphase Modeling of Transport Phenomena
in Spray-Drying Processes
Maksim Mezhericher,1 Avi Levy,2 and Irene Borde2
1
Center for Engineering Modeling, Design and Numerical Simulations,
Department of Mechanical Engineering, Shamoon College of Engineering, Beer-Sheva, Israel
2
Pearlstone Centre for Aeronautical Engineering Studies, Department of Mechanical Engineering,
Ben-Gurion University of the Negev, Beer-Sheva, Israel
Downloaded by [Ben Gurion University of the Negev] at 09:34 10 January 2015

occur on multiple scales and include simultaneous external


Spray drying is an extensively used technology in process engin- and internal heat and mass transfer in each phase.
eering for receiving small particles by rapid moisture evaporation Therefore, studies of spray drying supported solely by
from a spray of droplets. This contribution summarizes achieve- experimental measurements without modeling would be
ments and results of the comprehensive scientific research on insufficient and unable to encompass all of the encountered
multi-scale multiphase modeling of transport phenomena in
spray-drying processes undertaken by our research group: (1) study physical processes, predict parametric behavior, and
of particle formation on the scale of an individual droplet; (2) optimize the energy-consuming technology of spray drying.
modeling and simulation of droplet–droplet and particle–particle On the other hand, realistic modeling and numerical simu-
collisions in a spray; (3) study of gas-spray mixing; (4) 2D and lation of spray drying are important for choosing suitable
3D study of spray drying by an innovative multi-scale simulation operating conditions, but they still remain highly demand-
tool coupled to a commercial CFD software. The proposed
multi-scale multiphase model of transport phenomena in a ing tasks for engineers designing spray-dryer systems.[1–16]
spray-drying process has been developed based on a thorough analy- Computational Fluid Dynamics (CFD) is a popular
sis of previously published experimental and theoretical works. The technique utilized for modeling and numerical simulation
content of this paper will be useful for both academia and industry; of spray-drying processes.[17–21] This contribution sum-
e.g., pharmaceutical, biotechnology, chemical, ceramics, materials, marizes the modeling developments on multi-scale multi-
nutrition, and other applications of spray drying.
phase modeling of transport phenomena in spray-drying
processes contributed by our group over the years: (1)
Keywords CFD; Drying kinetics; Particle engineering; Spray
drying; Transport phenomena study of particle formation on the scale of an individual
droplet; (2) modeling and simulation of droplet–droplet
and particle–particle collisions in a spray; (3) study of
INTRODUCTION
gas-spray mixing; (4) 2D and 3D study of spray drying
Particle-formation technologies are utilized today in
by an innovative multi-scale simulation tool coupled to a
many areas, including pharmaceutical, medical and biome-
commercial CFD software.
dical, biotechnology, chemical, optical and optoelectronic,
cosmetic, printing, painting, ceramics, materials design,
nutrition, and other applications. Spray drying is con- THEORETICAL MODELING
sidered a suitable process for handling delicate biotechno- DROPLET SCALE: THERMO-PHYSICAL THEORY OF
logical products because it allows fabrication of small DRYING KINETICS OF A SINGLE DROPLET
particles by rapid moisture evaporation from a spray of The theoretical modeling of the spray-drying process is
droplets. The process involves multiphase transport based on a description of drying kinetics of individual
phenomena between drying agent, droplets and particles, droplets and particles. The drying kinetics of an individual
and chamber boundaries. These transport phenomena droplet containing solids (suspended or dissolved) is usually
divided into two drying stages. In the first drying stage, the
Correspondence: Avi Levy, Mechanical Engineering, Ben- droplet with excess liquid is subjected to a stream of drying
Gurion University of Negev, P.O.B. 653, Beer Sheva 84105,
Israel; E-mail: avi@bgu.ac.il gas (air, steam, nitrogen, etc.), gains sensible heat, and vapor-
Color versions of one or more of the figures in the article can ization begins. The evaporation results in droplet shrinkage
be found online at www.tandfonline.com/ldrt. and a simultaneous increase of solids concentration near

2
MULTI-SCALE MULTIPHASE MODELING 3

the droplet surface. In turn, this leads to the precipitation of a The mathematical description of single-droplet drying
solid component at the droplet surface and, eventually, all of kinetics is subsequently incorporated into a general drying
the surface becomes covered with a solid layer, called a crust. model of a spray comprising millions of droplets. The
At this moment, the droplet turns into a wet particle and the realistic model has to account for the complex physics of
second stage of drying commences. In the second stage, the spray drying, including reciprocal interactions between
drying process is hindered by additional resistance to evapor- drying agent (gas), liquid (droplets), and solid phases
ation posed by the crust layer. The second drying stage con- (particles). In turn, each phase is not a pure substance but
tinues until the particle moisture content reduces to is a mixture of several components. In this way, for all of
equilibrium with the drying medium. After this point, the the phases in the drying chamber, both internal (intra-
drying process actually stops and the particle is heated up droplet=particle) and external (gas-droplet=particle mixing)
to the thermal equilibrium temperature. Typical evolutions transport phenomena have to be taken into account. The
of droplet temperature and moisture content during the dry- theoretical modeling of such a system is rather challenging
ing process are outlined in Fig. 1. In this figure, the interval until some general simplifications are imposed. A reason-
between points 0 and 1 is corresponding to the droplet initial able assumption is to consider the drying gas as a continu-
heating; the period among points 1 and 2 is related to the ous phase and to treat the spray as a discrete phase, as far as
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droplet evaporation period; the interval among points 2 in spray dryers the gas phase occupies substantially greater
and 3 is related to the second drying stage; and finally, the volume compared to the dispersed droplets and particles.
period between points 3 and 4 designates the particle heating The concept of two-stage droplet drying kinetics is
up to equilibrium with the surrounding drying agent. illustrated by Figs. 1 and 2. One can identify three basic
morphological states of dispersed phase in a spray cham-
ber: droplets, wet particles with crust and wet core regions
and, finally, dry particles.
First Drying Stage
Droplet Initial Heating
The droplet initial heating-up is a quick process that
usually continues for less than tenths of a second in real
industrial conditions. This means that, during this period,
the drying character is unsteady and the value of Fourier
number, Fo ¼ ad t=R2d , can attain values less than 0.1.
Therefore, temperature distribution within the droplet should
be taken into account. Consequently, for a spherical droplet
with isotropic properties, the equation of energy conservation
is given by (intra-droplet liquid convection is neglected):
 
@Td 1 @ 2 @Td
qd cp;d ¼ 2 kd r ; ð1Þ
@t r @r @r

and the corresponding boundary conditions are:


8
< @Td
¼ 0; r ¼ 0;
@r ð2Þ
: hT  T  ¼ k @Td ; r ¼ R :
g d d @r d

The droplet outer radius, Rd, is considered to be unchange-


able due to insignificant evaporation. The value of heat
transfer coefficient, h, is determined using a well-known
Ranz-Marshall correlation[22]:
1=2
Nud ¼ 2 þ 0:6Red Pr1=3 : ð3Þ

The droplet specific heat can be evaluated as[23]:


 
@qt
FIG. 1. Typical drying curves of: (a) droplet temperature (solid line: cp;d ¼ þcp;w ð1  cÞ þ cp;s c: ð4Þ
@T p
suspension; dash line: solution); (b) droplet moisture content.
4 MEZHERICHER ET AL.
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FIG. 2. Single droplet drying in first stage (a) and second stage (b), (c).[29]

For ideal solutions and mixtures, considered here, the number can attain a value greater than 0.1, even at the
heat of mixing qt ¼ 0. The mass concentration of solids, beginning of the process. In this case, when the value of
c, is connected to the droplet moisture content, X, by: Biot number is less than 0.1, then the droplet lumped heat
capacity can be assumed and the droplet temperature
c ¼ 1=ð1 þ XÞ: ð5Þ depends only on time. Otherwise, the droplet temperature
must be treated as a function of both temporal and radial
The droplet density can be determined as follows: coordinates during the droplet evaporation. These two
  approaches for droplet temperature calculation are dis-
qd ¼ ð1 þ XÞqd;s qd;w = qd;w þ X qd;s : ð6Þ cussed below.
The uniform temperature approach is based on assump-
To find the droplet thermal conductivity, either series (7) tion of constant equilibrium evaporation temperature of
or parallel (8) conceptions are applied[24]: the droplet that is established in the droplet evaporation
period. This results in the following equation of energy
kd ¼ dkw þ ð1  dÞks ; ð7Þ conservation:

 
1=kd ¼ d=kw þ ð1  dÞ=ks ; ð8Þ _ v ¼ h Tg  Td Ad :
hfg m ð10Þ

where the droplet void fraction, d, is given by: The rate of mass transfer from the droplet surface is
  determined as follows:
d ¼ Vd;w =Vd ¼ 1  6md;s = pqd;s d3d : ð9Þ
 
m_ v ¼ hD qv;s  qv;1 Ad : ð11Þ
Since the droplet density, specific heat, and thermal
conductivity are functions of temperature, the solution of Combining (10) and (11), we get:
Eqs. (1)–(9) is obtained with the help of numerical methods.
   
hD qv;s  qv;1 ¼ h Tg  Td =hfg : ð12Þ
Liquid Evaporation from Droplet Surface
During liquid droplet evaporation from the droplet The coefficients of heat and mass transfer are determined
surface in the first drying stage (see Figs. 1 and 2a), Fourier by the corresponding Nusselt and Sherwood numbers,
MULTI-SCALE MULTIPHASE MODELING 5

which are evaluated using the modified Ranz-Marshall the droplet is turned into a wet particle) can be calcu-
correlations for evaporating spherical droplets[25]: lated as:
qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
ffi
dd h  1=2
dd;cr ¼ dd;0 3 qd;0 ð1 þ Xcr Þ= qd;cr ð1 þ X0 Þ : ð21Þ
Nud ¼ ¼ 2 þ 0:6Red Pr1=3 Þð1 þ BÞ0:7 ; ð13Þ
kd
For droplet with insoluble solids qw,cr  qw,1, Eq. (21)
dd hD  1=2

can be rewritten:
Shd ¼ ¼ 2 þ 0:6Red Sc1=3 ð1 þ BÞ0:7 ð14Þ
Dv qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
   
dd;cr ¼ dd;0 3 qd;w1 þ Xcr qd;s = qd;w1 þ X0 qd;s : ð22Þ
The factor (1 þ B)0.7 takes into consideration Stefan flow
in the droplet boundary layer and B ¼ cp,v(Tg  Td)=hfg is
known as the Spalding number. The rate of droplet mass change is found by combining
Combining Eqs. (12), (13), and (14) and treating both Eqs. (11), (14), (18), and (19):
vapor and drying air as ideal gases, the following equation  
is obtained: m _ v ¼ 0:5qd;w pdd C1 2 þ C2 d0:5
_ d ¼ m d : ð23Þ
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1=2   The droplet moisture content can be evaluated as follows:


Tg  Td 2 þ 0:6Red Sc1=3 Dv Mw pv;s pv;1
¼  : ð15Þ
hfg 1=2
2 þ 0:6Red Pr1=3 kg < Td Tg X ¼ md ð1 þ X0 Þ=md;0  1: ð24Þ

The droplet mass can be calculated by integrating Eq. (16):


This expression allows the evaluation of the droplet
equilibrium evaporation temperature.  
In order to calculate the droplet shrinkage rate, it is md ¼ md;0  pqd;w d3d;0  d3d =6: ð25Þ
assumed that elementary droplet mass decrease is pro-
portional to elementary droplet diameter shrinkage; i.e.,[26]: For drying air at atmospheric pressure, the coefficient
of vapor diffusion can be evaluated as follows[27]:
d ðdd Þ 2
¼ _ v:
m ð16Þ Dv ¼ 3:564  1010 ðTd;s þ Tg Þ1:75 : ð26Þ
dt qd;w pd2d

Combining (11) and (16) together with the Reynolds Note that here the temperatures are in Kelvin.
number definition, Red ¼ ugdg=vg, and expressing the mass In the case when both lumped heat capacity conditions,
transfer coefficient, hD, from Eq. (14), we have: Bi < 0.1 and Fo  0.1, are not satisfied simultaneously for
the dried droplet, the temperature profile within the droplet
must be taken into account. Consequently, for the droplet
d ðdd Þ 2 þ C2 d0:5
d
¼ C1 ; ð17Þ evaporation period, the energy conservation is described by
dt dd Eq. (1) when applied to the time-dependent spatial domain
0  r Rd (t). The corresponding boundary conditions for
where
this domain are given by:
 
C1 ¼ 2Dv qv;s  qv;1 =qd;w ð1 þ BÞ0:7 ; ð18Þ 8
> @T
< d ¼ 0; r ¼ 0;
C2 ¼ 0:6ðug =vg Þ1=2 Sc1=3 : ð19Þ @r ð27Þ
  _
: h Tg  Td ¼ kd @Td þ hfg mv ;
> r ¼ Rd ðtÞ:
For droplets with insoluble solids qv,s ¼ f(Td), and there- @r Ad
fore in equilibrium evaporation period qv,s ¼ const since
Td ¼ const. In such case the expression (17) can be inte- For the set of Eqs. (1) and (27), the value of the droplet
grated to give the duration of the evaporation period: outer radius, Rd (d), is tracked by a combination of Eqs.
(11) and (16).
 In contrast to the approaches suggested in the present
1   2 2  1:5 1:5

sep ¼ C 2 2C 2 dd;1  d d;cr  C2 d d;1  d d;cr study (the first approach assumes droplet temperature
C1 C42 3
profile during initial heating-up and then uniform droplet
 
ð20Þ
0:5 0:5
2 þ C2 d0:5
d;1 equilibrium temperature during evaporation period; the
 8 dd;1  dd;cr þ 16ln : second approach supposes non-uniform droplet tempera-
2 þ C2 d0:5
d;cr
ture in both periods of the first drying stage), the literature
The droplet diameter in the critical drying point (when survey of published models shows that a typical way is
the critical moisture content remains in the droplet and to assume a uniform droplet temperature profile in both
6 MEZHERICHER ET AL.

periods of the first drying stage. This point of view is based strength, and this duration can reach up to 32% from the
on the estimation that, in spray drying, droplet diameters overall duration of the first drying stage for the case of
are typically smaller than 1 mm and, therefore, the corre- nanosuspension droplet drying.
sponding Biot number is usually less than 0.1. As a result,
the ordinary differential equation of energy conservation
for this case is as follows[28]: Second Drying Stage
From the moment when droplet moisture content
dTd   decreases to the critical value, the process of porous crust
_ v þ cp;d md
hfg m ¼ h Tg  Td Ad : ð28Þ formation begins. Consequently, the droplet can no longer
dt
be treated as a liquid droplet, and it is considered to be a
A generally accepted approach to determine the moment wet particle consisting of a dry porous crust surrounding
of transition from the first to the second drying stage is a wet core. The outer diameter of the wet particle can be
to assume that this transition coincides with the moment assumed to be constant. At the same time, the internal
of initial crust formation on the droplet surface.[29] The particle wet core shrinks because of drying and the crust
corresponding value of the average droplet liquid fraction thickness increases. The wet particle drying can be
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is known as critical moisture content. The critical moisture classified as a problem with internal moving evaporating
content is usually determined by experiments, but for a interface (see Fig. 2b).
special case when, at the end of drying, a full porous The crust region of the wet particle can be treated as a
particle without any additional internal voids (cavities) lump pierced by a large number of identical, straight cylin-
will be formed, and an analytical formula for the droplet drical capillaries. It is also acceptable to consider the wet
critical moisture content can be developed: particle as a sphere with isotropic physical properties and
temperature-independent crust thermal conductivity. These
qw e assumptions lead to the following equation of energy
Xcr ¼ ð29Þ conservation for the crust region:
qs 1  e
 
The distinction between two different drying stages and @Tcr acr @ 2 @Tcr
¼ 2 r ; Ri ðtÞ  r  Rp ; ð31Þ
respective droplet morphology states is given by the @t r @r @r
following criterion:
and the corresponding boundary conditions are:
8
< Xd  Xcr ; first drying stage ! droplet; 8
Xd : Xf < Xd < Xcr ; second drying stage ! wet particle; >
> @Tcr @Twc _v
m
:
Xd ¼ Xf ; final sensibe heating ! dry particle: < kcr @r ¼ kwc @r þ hfg A ; r ¼ Ri ðtÞ;
>
i
ð32Þ
ð30Þ >
> T wc ¼ T cr ; r ¼ R i ð t Þ;
: hT  T  ¼ k @Tcr ; r ¼ R :
>
g cr cr @r p
In the above equation, Xf is the final (bounded) moisture
content of dry particle.
Recently, a more sophisticated approach to determine Note that the droplet temperature at the point of critical
the duration of the first drying stage has been proposed moisture content is taken as an initial condition for
by Mezhericher et al.[30] As the result of liquid evaporation Eq. (31).
from the droplet surface, concentration of solids on the The rate of vapor mass transfer from the particle outer
surface continuously increases and, at some time moment, surface is determined according to Eq. (11), but the droplet
it reaches saturation. A thin layer of crust appears on the surface area, Ad, is substituted for the particle surface area,
droplet surface. This initial layer is unstable and collapses Ap. The mass of particle crust is calculated using the
due to compressive capillary forces.[30] After the collapse, expression:
ongoing evaporation leads to renovation and thickening  
of the crust layer. If this newly formed crust is not yet thick mcr ¼ 4=3pð1  eÞqcr;s R3p  R3i : ð33Þ
enough to withstand compressive capillary pressure, it
buckles again. The loop of crust formation and crust buck- The coefficient of vapor diffusion at particle surface
ling repeats itself until the crust will be thick enough to is determined by Eq. (26).
withstand the capillary pressure. The period of repetition For the region of the particle wet core, the equation of
of the evaporation and shell collapsing at the end of the energy conservation is as follows:
first drying stage is known as transition period.[30–32] Recent  
@Twc 1 @ @Twc
theoretical studies[33] have demonstrated that the duration qwc cp;wc ¼ 2 kwc r2 ; 0  r  Ri ðtÞ: ð34Þ
of the transition period strongly depends on the crust @t r @r @r
MULTI-SCALE MULTIPHASE MODELING 7

The corresponding boundary conditions: Summarizing (33), (39), and (42), the mass of wet particle
8 @Twc can be calculated:
< @r ¼ 0; r ¼ 0;
> !
md;0 qwc;w 4 h i
_v
m
kcr @T @Twc
@r ¼ kwc @r þ hfg Ai ; r ¼ Ri ðtÞ;
cr ð35Þ mp ¼ 1 þ pqwc;w eR3i þ ð1  eÞR3p :
>
: 1 þ X0 qwc;s 3
Tcr ¼ Twc ; r ¼ Ri ðtÞ:
ð43Þ
The position of the crust-wet interface is given by[26]:
The thermophysical properties of the particle crust
d ðR i Þ 1 region are determined by considering it as a porous medium.
¼ _ v:
m ð36Þ
dt eqwc;w 4pR2i In this way, the crust thermal conductivity is given by:

In the present study, it is assumed that the crust pore kcr ¼ kcr;s ð1  eÞ þ e kcr;g : ð44Þ
diameter is much greater than the mean free path of vapor
molecules (i.e., the corresponding value of Knudsen The crust density is evaluated as follows:
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number, Kn ¼ kv=dc, is substantially less than unity).


Consequently, the process of vapor diffusion in the crust qcr ¼ qcr;s ð1  eÞ: ð45Þ
pores is treated as independent of pore size and governed
only by vapor concentration gradient. As a result, each Typically, values of specific heat of solids, cp,s, and
crust pore can be considered as a semi-open Stefan’s system specific heat of drying agent, cp,g, are of the same order;
and the mass transfer rate from a spherical wet particle can therefore, for these cases, the crust specific heat is equal
be calculated according to the following equation[28]: to that of the solids; i.e., cp,cr  cp,s.
For particle wet core, the specific heat and thermal conduc-
8peb Dv;cr Mw pg Rp Ri
_v ¼ 
m  tivity are determined by Eqs. (4) and (7) or (8), respectively.
< Tcr;s þ Twc;s Rp  Ri
2 3
pg  pv;i ð37Þ Drying of Single Droplets Containing Dissolved Solids
6   7 In the case of drying of single droplets with dissolved
 ln4 p 5:
pg  4pM <h R2 m _ v þ Tv;1
g
Tp;s solids, the reaction engineering approach[34] can be utilized.
w D p
According to this approach, partial vapor pressure over the
surface of the droplet with dissolved solids depends not
Here, the coefficient of vapor diffusion in the crust pores, only on temperature, but also on the droplet moisture con-
Dv,cr, is calculated using Eq. (26). tent. The density of vapor over the surface of the solution
The particle moisture content is given by: droplet can be found as follows:
X ¼ mp ð1 þ X0 Þ=md;0  1: ð38Þ  
qv;s ¼ wqv;sat Td;s : ð46Þ
The mass of solid component in the particle wet core can be
determined as follows: The fractionality, w, and apparent activation energy,
DEv, are calculated by:
 
mwc;s ¼ md;0 =ð1 þ X0 Þ  4=3pð1  eÞqcr;s R3p  R3i : ð39Þ  
w ¼ exp DEv = < Td;s ; ð47Þ
The density of particle wet core is evaluated with the help  
DEv ¼ a  DEv;g exp½b Xd  Xg Þc ; ð48Þ
of Eq. (6). The wet core mass is equal to:

mwc ¼ 4=3pqwc R3i : ð40Þ where a, b and c are empirical coefficients; Xd and Xg are
corresponding moisture contents of the droplet and drying
Combining (6), (39), and (40), the mass of wet core can be ambient. The apparent activation energy for drying agent
obtained: (air), DEv,g, is given by:
   
mwc ¼ mwc;s þ qwc;w =qwc;s 4=3pR3i qwc;s  mwc;s : ð41Þ DEv;g ¼ <Tg ln qv;1 =qv;sat Tg : ð49Þ

Assuming that drying air is an ideal gas, we can obtain:


Correspondingly, the mass of liquid fraction in the particle
wet core is given by:  
DEv;g ¼ <Tg ln ug ; ð50Þ
 
mwc;w ¼ qwc;w =qwc;s 4=3pR3i qwc;s  mwc;s : ð42Þ where ug is the gas relative humidity.
8 MEZHERICHER ET AL.

Drying-Induced Stresses in Wet Particles rh;tot ðr; tÞ ¼ rT;h ðr; tÞ þ rh ðr; tÞ: ð58Þ
As the result of drying of wet particles in the second
drying stage of the spray-drying process, temperature These total stresses can lead to cracking=rupture of wet
differences across the crust region can lead to the appear- particles during drying, if they are greater than the crust
ance of thermal stresses.[35,36] The radial, rT,r, and tangential strength. The corresponding criterion for particle damage
rT,h, thermal stresses in the porous crust of a wet particle are is as follows[36]:
calculated by assuming that the crust inner and outer     
surfaces have free radial strains[37]: max rr;tot ; max rh;tot  ½rt ; ð59Þ
2aT;cr Ecr
rT;r ðr; tÞ ¼ where [rt] is crust tensile strength.
ð1  ncr Þr3
2 3
3 3 ZRp Zr CHAMBER SCALE: MULTIPHASE FLOW OF SPRAY
6 r  Ri  7
 4 s2 Tcr ðs; tÞds  s2 Tcr ðs; tÞds5; AND DRYING AGENT
3 3
Rp  Ri R
i R i The multiphase flow of drying agent and spray of
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ð51Þ droplets in a drying chamber is treated by the Eulerian-


Lagrangian approach. The governing equations for the
aT;cr Ecr continuous gas phase (drying agent) include continuity,
rT;h ðr;tÞ ¼ momentum, energy, and species conservations. The effect
ð1ncr Þr3
2 3 of turbulence is typically encountered by means of the k-e
Rp
3 3 Z Zr model, which was verified to be suitable for a satisfactory
62r þRi 7
4 3 s2 Tcr ðs; tÞdsþ s2 Tcr ðs; tÞdsr3 Tcr ðr; tÞ5: description of air flow-fields in spray dryers and laying
Rp R3i
Ri Ri down low demands on computational resources.[21]
The recent advances in describing the different levels of
ð52Þ
turbulence in the spray drying chambers are reported
The Young modulus for the porous crust can be elsewhere.[39,40]
determined as follows[38]: The dispersed phase (spray of droplets and particles)—
trajectories of spray droplets=particles and their essential
  parameters—are calculated using a Discrete Phase Model
Ecr ¼ C1 Es;0 1  am Tcr =Tm;s ð1  eÞn : ð53Þ
(DPM) formulated in Lagrange moving reference frame
(the basic ideas of DPM for sprays can be found in the
In addition to thermal stresses, pressure difference
publications of O’Rourke[41,42] and Crowe et al.[43]). A
across the crust region leads to the appearance of mechan-
turbulent dispersion of the discrete phase is currently disre-
ical stresses in wet particles.[36] The radial and tangential
garded. The motion of the droplets=particles is described
mechanical stresses in the porous crust[37]:
by Newton’s Second Law, including drag, buoyancy,
  pressure gradient, contact and other forces (e.g., phoretic,
R3i R3p  r3 Basset, Saffman, Magnus forces, etc.[43]).
rr ðr; tÞ ¼ Dpcr  ; ð54Þ
r3 R3p  R3i
Continuous Phase
  The continuous phase of drying gas is treated by a
R3i 2r3 þ R3p Eulerian approach and a standard k-e model is utilized
rh ðr; tÞ ¼ Dpcr  : ð55Þ for the turbulence description. The utilized conservation
2r3 R3p  R3i equations of continuity, momentum, energy, species, tur-
bulent kinetic energy, and dissipation rate of turbulence
Here, the pressure difference across the particle crust is: kinetic energy are as follows[44] (i, j ¼ 1, 2, 3):
continuity
Dpcr ¼ pðtÞjr¼Ri pg ð56Þ

Total stresses in the radial and tangential directions are @q @  


þ quj ¼ Sc ð60Þ
the sums of the corresponding thermal and mechanical @t @xj
stresses:
where q and u are drying gas density and velocity, and
rr;tot ðr; tÞ ¼ rT;r ðr; tÞ þ rr ðr; tÞ; ð57Þ Sc is mass source term.
MULTI-SCALE MULTIPHASE MODELING 9

momentum conservation where T is gas temperature and b is coefficient of gas


thermal expansion:
    
@ @   @p @ @ui @uj 1 @q
ðqui Þþ qui uj ¼  þ l þ b¼ ð68Þ
@t @xj @xi @xj e @xj @xi q @T p
;
þDqgi þUpi Sc þRFgp ð61Þ
The recommended constants are C1 ¼ 1.44, C2 ¼ 1.92, and
the Prandtl numbers are equal to rk ¼ rh ¼ rY ¼ rT ¼ 0.9
where p and le are drying gas pressure and effective and re ¼ 1.3. The effective viscosity, le, is defined as:
viscosity, Up is particle velocity, and RFgp is sum of
the forces exerted by particles on gas phase. le ¼ l þ lT ; ð69Þ
energy conservation (thermal radiation to the gas where lT is turbulent viscosity
phase is neglected)
k2
  lT ¼ Cl q : ð70Þ
@ @   @ le @h e
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ðqhÞ þ quj h ¼ þ Sh ; ð62Þ


@t @xj @xj rh @xj Here, Cl ¼ 0.09.
The constitutive relationship between air temperature,
where h is specific enthalpy and Sh is energy source pressure, and density is given by the ideal gas law (such
term. assumption is sufficient because of the small humidity of
the gas involved in the considered multiphase flow; more
species conservation details can be found in the further sections):
  q
@ @ @ le @Yv p ¼ <T; ð71Þ
ðqYv Þ þ ðquj Yv Þ ¼ þ Sc ; M
@t @xj @xj rY @xj
where < is universal gas constant and M is molecular
ð63Þ
weight of the gas phase.
where Yv is mass fraction of vapor in humid gas. Discrete Phase
As it was previously mentioned, to track the trajectories
turbulence kinetic energy and other valuable parameters of the spray of droplets and
  particles, a Discrete Phase Model (DPM) based on Lagran-
@ @   @ le @k
gian formulation is utilized.[41–43,45–47] The motion of
ðqkÞþ quj k ¼ þGk þGb qe;
@t @xj @xj rk @xj droplets=particles is described by Newton’s Second Law:
ð64Þ P~
~p
dU Fp
¼~ gþ : ð72Þ
where k is turbulent kinetic energy and e is dissipation dt mp
P~
rate of turbulent kinetic energy. Here, Fp is the sum of the forces exerted on a given
spray droplet=particle by the gas phase, by other particles
dissipation rate of turbulence kinetic energy
and walls of the spray drying chamber; mp is particle mass
  and ~g is gravity acceleration. In general, the acting forces
@ @   @ le @e e
ðqeÞþ quj e ¼ þ ðC1 Gk C2 qeÞ on the spray droplet=particle are:
@t @xj @xj re @xj k
X
ð65Þ ~
Fp ¼ ~
FD þ ~
FB þ ~
FA þ ~
FPG þ ~
FC þ ~
Fother ; ð73Þ

Note that in Eq. (64) the production of turbulence kinetic where ~ FD is drag force, ~
FB is buoyancy force, ~
FA is added
energy due to mean velocity gradients is equal to: ~
mass force, FPG is pressure gradient force, and ~ FC is con-
  tact force. The term ~ Fother represents other forces, usually
@ui @uj @ui important for submicron particles and=or at specific con-
Gk ¼ l T þ ; ð66Þ
@xj @xi @xj ditions (e.g., phoretic, Basset, Saffman, Magnus forces,
and the production of turbulence kinetic energy due to etc.[43]), which are neglected in the present work.
buoyancy is given by: The drag force is determined by the expression[48]:

lT @T pd2p   
Gb ¼ bgj ; ð67Þ ~  ~ p  ~ ~p ;
rT @xj FD ¼ qCD ~uU uU ð74Þ
8
10 MEZHERICHER ET AL.

where dp is particle diameter. The drag coefficient, CD, is the interaction. The particles are assumed to be spherical,
calculated according to known empirical correlations for quasi-rigid, and their shapes are retained after impact.
spherical particles.[49] Furthermore, quasi-instantaneous contact between two
The buoyancy force, ~ FB , opposes gravity and in the colliding particles is considered to occur at a point (see
present study it is much smaller than the latter, because Fig. 3).
the densities of spray droplets and drying gas differ more The probabilistic algorithm for detection of binary
than a thousand times. For this reason, the buoyancy of collisions allows dealing with a large number of droplet–
droplets=particles is currently neglected. droplet and particle–particle interactions encountered
The added mass (‘‘virtual-mass’’) force, required to in spray towers. To reduce the cost of computations for
accelerate the gas surrounding the droplet=particle, is systems with many droplets and particles, this approach
given by[43]: proposes a probabilistic concept of collision between
droplet=particle parcels instead of dealing with individual
pd3p d   objects.[43] A droplet=particle parcel represents a group
~
FA ¼ q ~ ~p :
uU ð75Þ of droplets=particles with the same properties, such as
12 dt
diameter, position, velocity, etc., and there are no interac-
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For flow in spray dryers, this force may be important in the tions between the droplets=particles inside the parcel. The
region of spray injection, where the velocities of injected droplet=particle parcel behaves like individual droplets=
spray droplets and drying gas are substantially different particles with mass equal to the mass of all droplets=
and intensive gas-droplet mixing leads to high change rates particles of the parcel. For convenience, collisions
of the gas-droplet relative velocities. between two droplet parcels and collisions between
The pressure gradient in the gas phase additionally two particle parcels are referred to as droplet–droplet
accelerates droplets=particles and results in the following and particle–particle collisions, correspondingly. It is
force[43]: worth noting that in spite of several known disadvantages
of the adopted probabilistic method, its choice is justified
pd3p ~ by the significant benefits: the algorithm is consistent with
~
FGP ¼  rp ð76Þ stochastic nature of spray behavior and it is of
6
second-order accuracy in space.[54,55]
This force can be essential and is worth consideration
in the spray dryer regions with fast pressure changes,
such as the inlet, outlet, and swirling zones of the gas
phase.
The contact force, ~FC , arises from collision interactions
between the given droplet=particle with other droplets=
particles or walls of the drying chamber. For calculation
of droplet–droplet and particle–particle collisions in spray
dryers, a novel stochastic model has recently been
proposed.[50] Several assumptions have been utilized in
this theory. To simplify the model and facilitate the calcu-
lations, rotational motions and plastic deformations of
the particles are neglected. Also, electrostatic forces
arising from friction between two colliding particles are
not taken into account. Breakage of particles due to colli-
sions is not modeled. No agglomeration or adhesion
between particles is considered, so only bouncing of
colliding particles is assumed. Droplet–particle interac-
tions are neglected and only binary (one-on-one) drop-
let–droplet and particle–particle collisions are taken into
account. The particle–particle collisions are described by
applying a hard-sphere approach of discrete particle inter-
actions,[51,52] combined with a probabilistic algorithm of
collision detection[41,45,53] used earlier only in the studies FIG. 3. Scheme of binary particle–particle collision. (Reprinted
with permission from International Journal of Multiphase Flow, Vol. 43,
involving droplet–droplet interactions. In the hard-sphere Mezhericher, M.; Levy, A.; Borde, I. Probabilistic hard-sphere model of
approach, the collision forces are considered as impulsive binary particle–particle interactions in multiphase flow of spray dryers,
and all other forces are considered to be negligible during pp. 22–38, 2012, with permission from Elsevier.)
MULTI-SCALE MULTIPHASE MODELING 11

Droplet–Droplet Collisions mean expected number of collisions can be obtained from


The droplet–droplet collisions in sprays are usually Eq. (79):
treated by stochastic mathematical methods. One of the
widely known approaches is the O’Rourke model,[41]  ¼ ln 0:5 ¼ 0:69315
n ð80Þ
which benefits from the ability to deal with a large
amount of simultaneous droplet–droplet interactions The above relation represents the criterion for detecting the
for reduced computational costs by implementing a acts of droplet collisions during numerical simulations: if
concept of collisions between droplet parcels and not n  ncr , then the collision occurs reliably.
individual droplets.[43] The algorithm of the O’Rourke The droplet behavior after the collision depends on the
probabilistic model is consistent with the stochastic type of the collision: bounce or coalescence (breakage of
nature of sprays and it is of second-order accuracy in colliding droplets is not considered in this study). The
space.[54,55] In addition, the O’Rourke method has been outcome of the collision will to be a coalescence of the
implemented in Computational Fluid Dynamics (CFD) two droplet parcels if they collide head-on, and a grazing
code ANSYS FLUENT, which facilitated the numerical collision occurs if the parcels collide in a more oblique
way. The type of collision is determined based on spatial
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simulations of droplet–droplet interactions undertaken


in our previous studies of multiphase flow in spray offset between the two parcels immediately before the
dryers.[45,46] collision:
According to O’Rourke, the droplets of the same pffiffiffiffiffiffiffi
b ¼ ðr1 þ r2 Þ Rm ; ð81Þ
parcel do not interact with each other, only with the
droplets of the other parcels. It is assumed that the where Rm is a random number between 0 and 1. This offset
droplet parcel behaves in spray like an individual is then compared to the critical collisional offset:
droplet with mass, mechanical, and thermal energies equal
to the total mass and the energies of all of the droplets in sffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
 
the parcel. 24f ðr1 ; r2 Þ
bcr ¼ ðr1 þ r2 Þ min 1:0; ; ð82Þ
Two droplet parcels simultaneously crossing the same Wec
cell of the numerical grid are likely to collide. Let us
designate the parcel of bigger droplets as ‘‘collector’’ (con- where the function f and the collision Weber number,
tains n1 droplets) and another parcel of smaller droplets is Wec, are given by:
labelled as ‘‘contributor’’ (contains n2 droplets). Then, a
mean expected number of collisions for the collector, n, is  3  2  
r1 r1 r1
given by: f ðr1 ; r2 Þ ¼ 2:4 þ2:7 ; ð83Þ
r2 r2 r2
n2 pðr1 þ r2 Þ2 ur Dt
n ¼ ; ð77Þ qu2r ðr1 þ r2 Þ
V Wee ¼ ð84Þ
r
where r1 and r2 are radii of the collector and the contributor,
Here, r is surface tension.
ur is relative velocity between the droplet parcels, Dt is
If b < bcr, then the collision results in coalescence of the
computation time step, and V is volume of numerical cell.
two droplet parcels, and each droplet from the collector
The probability of the number of collisions for the collector,
unites with a droplet from the contributor to form an
m, is assumed to obey the Poisson distribution:
agglomerate on a one-to-one basis. When there is an excess
nm
 of droplets in the contributor, this surplus remains in the
PðmÞ ¼ en : ð78Þ contributor and will be tracked at the next computational
m!
step. The velocities of the agglomerated parcel and the
The probability of at least one collision between the two remaining droplets in the contributor, as well as the corre-
considered parcels, P1 ¼ P(m  1), can be calculated as sponding contact forces, are determined using the law of
complementary to the probability of no collisions, momentum conservation and Newton’s Second Law of
P(m ¼ 0)[56]: Motion. After the coalescence, the collector radius
increases in accordance with the volume conservation:
P1 ¼ 1  Pðm ¼ 0Þ ¼ 1  en : ð79Þ
r31;new ¼ r31 þ r32 : ð85Þ
O’Rourke’s method considers that the collision
between two parcels occurs reliably when the probability If b > bcr, then the collision is grazing and it is assumed
of at least one collision exceeds the boundary value of that some portion of the droplet kinetic energy of
0.5; i.e., P1  0.5.[56] The corresponding critical value of translational motion is spent on viscous dissipation and
12 MEZHERICHER ET AL.

generation of angular momentum. The corresponding The post-collision velocity for each colliding particle
post-collision velocity of the droplet parcel can be calculated parcel is calculated by applying Newton’s Second and
as follows: Third Laws of Motion, and three additional theoretical
definitions of coefficients of normal restitution, e, dynamic
  friction, g, and tangential restitution, b0. The values
u þ mp;2~
mp;1~ u þ mp;2 ð~
u ~
uÞ b  bcr
u1; new
~ : ð86Þ of these coefficients are obtained experimentally. A brief
mp;1 þ mp;2 r1 þ r2  bcr
mathematical description of the utilized method of
particle–particle collisions is given below.
The vector of contact force, ~
Fc;1 , is given by:
For two colliding particles A and B (Fig. 3), a unit
vector in normal direction of the collison, n ^, can be
 
~
FC;1 ¼ mp;1 ~u1;new  ~
up;1 =Dt: ð87Þ established at their contact point:

For the second colliding parcel, ~


FC;2 ¼ ~
FC;1 , and its rA ~
~ rB

n ; ð88Þ
new velocity vector can be evaluated from Newton’s rA ~
j~ rB j
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Second Law.
where ~rA and ~
rB are radius-vectors of particles A and B,
respectively. Using Newton’s Second and Third Laws
Particle–Particle Collisions of Motion, the following set of equations can be
Evaporation of liquid from droplets eventually results in derived:
their transformation into wet particles. Correspondingly,
(  
droplet parcels turn into particle parcels. Particle–particle mA ~ vA;0 ¼ ~
vA  ~ J;
collision is detected if the moisture contents of the colliding   ð89Þ
mB ~ vB;0 ¼ ~
vB  ~ J:
parcels are less than critical moisture content. The collision
between particle parcels is referred to as particle–particle
interaction. where ~vA;0 and ~vB;0 are translational velocities of parti-
Mezhericher et al.[50] proposed to apply the O’Rourke cles before the collision, and mA and mB are their
probabilistic algorithm to detect particle–particle colli- masses, respectively. The momentum transferred during
sions along with droplet–droplet collisions. Correspond- the collision is given by the impulse vector:
ingly, Eq. (77) is utilized to predict the mean expected
ZDt
number of collisions for particle collector. If this value
~ ^ þ Jt^t ¼
J ¼ Jn n ~
FC ðtÞdt; ð90Þ
is greater than the critical number of collisions,
Eq. (80), the collision between two particle parcels occurs 0
definitely. To treat the particle–particle collisions and to
where Dt is collision duration, ~
FC is contact force (see
predict the post-collision state of the colliding pair,
Eq. (87)), and Jn and Jt are normal and tangential com-
Mezhericher et al.[50] suggested to utilize a hard-sphere
ponents of impulse vector, respectively. The relative
approach of discrete particle interactions. Hard-sphere
velocity at the contact point is determined as follows
(also hard particle) methodology was initially developed
(bearing in mind that rotation of particles is disre-
in the physics of molecular dynamics to numerically
garded in the present formulation):
study phase transitions in molecular systems.[57–60] Later
on, this technique was adopted for granular dynamics vAB
~
~ vA;c  ~
vB;c ¼ ~
vA  ~
vB ; ð91Þ
simulations.[61] Recent progress has enabled the
hard-sphere approach for calculation of particle–particle where ~vA;c and ~
vB;c are velocities of the particle parcels
interactions for dilute and dense gas-particle flow at the common contact point. Using Eq. (91), a unit
regimes.[21,43,51,52,62–81] vector in tangential direction of collision can be deter-
According to hard-sphere method, binary collisions mined:
between rigid spherical particles are considered. It is
assumed that only impulsive interaction forces are signifi-  
cant during the act of collision. Mezhericher et al.[50] vAB;0  ~
~ n~ vAB;0  ~
n
^t ¼    : ð92Þ
adapted the hard-sphere formulation developed by ~
vAB;0  ~
n~ n 
vAB;0  ~
Hoomans,[51] but rotational motions of particles were
disregarded and not included in the momentum equations. Combining Eqs. (89) and (91) yields:
In addition, Mezhericher et al.[50] considered binary colli-
sions between particle parcels, whereas Hoomans[51]
described the interactions between individual particles. ~ vAB;0 ¼ B2~
vAB  ~ J ð93Þ
MULTI-SCALE MULTIPHASE MODELING 13

where B2 ¼ m1A þ m1B . To complete the system of momentum It is worth noting that some portion of particle energy
equations (89), three additional empirical parameters are is dissipated during the act of collision and this energy
introduced: dissipation can be calculated knowing the coefficients
of restitution and dynamic friction (Eq. (94)–(96)). More
coefficient of normal restitution, 0  e  1:
details are given elsewhere.[50]
 
vAB  n
~ ^ ¼ e ~vAB;0  n
^ ; ð94Þ
CASE STUDIES
coefficient of dynamic friction, g  0: Spray Drying Chamber
    To perform the investigations of transport phenomena
  in a spray dryer using the developed model, three-
n^ ~
J ¼ g n^ ~
J ; ð95Þ
dimensional numerical simulations of drying behavior
coefficient of tangential restitution, 0  b0  1: of silica suspension droplets have been undertaken. The
studied droplets were atomized from the suspension of
  silica spherical particles in water with initial moisture
^ ~
n vAB ¼ b0 n^ ~
vAB;0 : ð96Þ
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content of 1.35 kg H2O=kg dry solid. The utilized silica


particles have size 272 nm and their density is 1950 kg=m3.
From Eqs. (93) and (94), the expression for normal In the numerical investigations, the porosity of the dry
component of impulse vector can be derived: crust consisting of identical silica nanoparticles was
assumed to be e ¼ 0.4 and the corresponding droplet critical
vAB;0  n
~ ^ moisture content, Xcr, was set to 0.34 kg H2O=kg solid in
Jn ¼ ~
Jn
^ ¼ ð1 þ eÞ : ð97Þ
B2 accordance with Eq. (29). The wet particles were dried until
their moisture decreased below the value of 0.05 kg H2O=kg
The calculation of tangential component of impulse solid. The basic operating characteristics and configuration
vector, Jt, depends on type of particle–particle collision: of the spray-drying setup (see Fig. 4) were adopted from
sticking or sliding. In a case when grazing collision occurs the literature.[82] A centrifugal pressure nozzle is located
during the collision, the collision is of the sliding type; at the top of the cylinder-on-cone drying chamber with
otherwise, the collision is of the sticking kind. Mathe- co-current flow. Hot atmospheric air flows into the chamber
matically, the following criterion is applied: through an annulus on the top horizontal ceiling and the air
velocity vector is directed at 35 with respect to the chamber
sliding particle–particle collision
vertical axis. The inlet air has temperature 468 K, humidity
0.009 kg H2O=kg, magnitude of inlet velocity 9.08 m=s,
vAB;0  ^t
ð1 þ b0 Þ~ turbulence kinetic energy 0.027 m2=s2, and turbulence energy
g< ; ð98Þ
Jn B1 dissipation rate 0.37 m2=s3. The cone angle of spray of
droplets is set to 76 , the magnitudes of droplet velocities
sticking collision between particles at the nozzle outlet are equal to 59 m=s, and initial spray
temperature is assumed to be 300 K. The spray of droplets
vAB;0  ^t
ð1 þ b0 Þ~ with mass flow rate equal to 0.0139 kg=s (50 kg=hr) is
g ; ð99Þ
Jn B1 simulated by assuming that the spread in atomized droplet
diameters obeys the Rosin-Rammler distribution in which
where B1 ¼ 72 B2 (see [51]). Correspondingly, for the 70.5 mm is the mean droplet diameter, 10.0 mm and
sticking collision we get: 138.0 mm are the corresponding minimum and maximum
    droplet sizes, and the spread parameter is 2.09. The walls
  n^ ~vAB;0 
~ ~ ~
Jt ¼ J  t ¼  n  J ¼  ð 1 þ b 0 Þ
^ of a spray dryer made of 2 mm stainless steel are assumed
B1 to be perfectly insulated. For the chamber outlet pipe, the
ð100Þ
^
vAB;0  t
~ gage air pressure is set equal to 100 Pa.
¼ ð1 þ b0 Þ :
B1
Numerical Simulations
And for the sliding collision we have: The numerical solution of the conservation equations
Jt ¼ gJn : ð101Þ for the continuous phase of drying gas has been performed
with the help of a 3D, pressure-based solver of CFD
Now, using Eqs. (89), (90), (97), (100), and (101), the package ANSYS FLUENT 13. The solver utilizes the finite
post-collision velocities of the colliding pair of particles volumes Euler-DPM numerical technique and benefits
can be determined. from a two-way coupling between the continuous (gas)
14 MEZHERICHER ET AL.

and discrete (droplets and particles) phases. Figure 5a,b the CFD code ANSYS FLUENT 13 via the mechanism
illustrates the utilized numerical grid, which consisted of of user-defined functions (UDFs).[29,50,83]
619,711 unstructured meshes of tetrahedral and polyhedral The general strategy of numerical simulations was
shapes. To compute the transport phenomena for the dis- as follows: first, the flow patterns of drying air were
crete phase according to the developed models of drying calculated without the presence of discrete phase and
kinetics and inter-particle collisions, original numerical sol- a converged solution was obtained; next, spray droplet
ution routines were developed, compiled, and attached to injections were introduced into the computational domain
and coupled air-spray calculations were performed.
Until now, Mezhericher et al.[29,47,50] have investigated
important aspects of transport phenomena in spray drying:
(1) influence of droplet–droplet and particle–particle colli-
sions on predicted transport phenomena in spray dryers—
unsteady-state numerical simulations using the developed
model of inter-droplet and inter-particle collisions and sim-
plified ‘‘pure water droplet’’ drying kinetics[45,50]; (2) study
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of drying kinetics of spray-drying processes—steady-state


numerical simulations utilizing a developed description of
droplet=wet particle drying kinetics and neglecting drop-
let–droplet and particle–particle interactions.[29,47]
In the first case study, accounting for both droplet–droplet
and particle–particle collisions, to simulate the nozzle atomi-
zation, 20 droplet streams were injected into the computa-
tional domain along the spray cone, as shown in Fig. 5c.
Through each droplet stream, 20 droplet parcels of different
diameters were introduced simultaneously, according to
the above-mentioned Rosin-Rammler distribution. In this
way, 400 new droplet parcels were injected into the cham-
ber at any gas flow time step. Any time the collision was
detected, its type was established based on the moisture
contents of the colliding pair. It is worth mentioning that
instances of droplet–particle collisions have been regis-
tered, though they have not been treated during the
numerical simulations.[50] The unsteady-state numerical
simulations of spray drying have been performed using
four-way coupling between the continuous and dispersed
phases. The convergence of unsteady numerical simula-
tions was established by monitoring the residuals of the
governing equations and demanding their negligible values
(at least smaller than 0.001) at each computational time
step. In the performed simulations, the fluid flow time step
was set to 0.1 s (determined as optimal by trial and error
method), and simulation of spray-dryer performance
during 30 consumed about a week of a continuous com-
puter run. To achieve the convergence, about 100 numeri-
cal iterations per fluid time step were required.
In the second case study, where the developed model of
droplet drying kinetics was enabled, the liquid spraying
was also simulated by introducing 20 spatial droplet
streams into the spray chamber (Fig. 5c). However, in
contrast, each droplet stream was represented by 10
injections of different droplet diameters, obeying the
Rosin-Rammler distribution. In this way, totally 200 dif-
FIG. 4. Spray drying unit: (a) sketch (dimensions are in mm); ferent droplet injections were simultaneously introduced
(b) isometric view.[29] into the computational domain. In addition, though in
MULTI-SCALE MULTIPHASE MODELING 15
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FIG. 5. Numerical grid and spray imitation: (a) XZ vertical section of 3D numerical grid; (b) surface mesh of the computational domain; (c) spray from
nozzle simulated by 20 injected droplet streams.[29]

this case droplet–droplet and particle–particle collisions For 2D and 3D patterns of air flow without spray
were disregarded, two possibilities of particle–wall interac- injection, the developed model has been validated by using
tions have been investigated: (1) particles hitting chamber the published experimental results on distribution of
walls ‘‘escape’’ from the computational domain; i.e., the velocity magnitudes in the adopted spray-drying set-up.[45,53]
droplets=particles trajectories were terminated if striking For 3D drying of wet particles (drying kinetics of the
against the dryer walls; (2) particles hitting the chamber walls second drying stage), the developed model has been vali-
rebounded from the walls with restitution coefficients dated by comparing the predicted and available from the
0.9 (normal) and 0.5 (tangential). The convergence of the literature experimental evolutions of air temperature and
steady-state numerical solutions was established using moisture of PVC wet particles in a pneumatic dryer.[85]
the residuals of the governing equations and, in addition, Despite the already undertaken successful validation
the overall imbalances between the domain incoming and studies, further research on the model validation is still
outgoing mass flow and heat transfer rates were monitored essential, especially by comparing the predicted and experi-
as well. The negligibly small values of the above parameters mental parameters of droplet and particle drying kinetics
were required to achieve the converged numerical solution. of three-dimensional spray-drying processes.

Validation Case Study 1: Droplet–Droplet and Particle–Particle


Until now, the developed model of the spray-drying Collisions
process has been validated several times. In the first of the two case studies given in the present
On the scale of single droplet=wet particle, the model of paper, influence of droplet–droplet and particle–particle
droplet drying kinetics has been validated by the authors collisions on predicted transport phenomena in spray
using the literature data on silica, skim and whole milk dryers has been investigated by means of unsteady-state
droplets,[35,83] and experimental drying characteristics of numerical simulations using the developed model of
acoustically levitated silica droplet.[31] Recently, Mortier inter-droplet and inter-particle collisions and simplified
et al.[84] carried out an in-depth independent study using ‘‘pure water droplet’’ drying kinetics.[45,50] To illustrate
the droplet drying kinetics described in this paper and their the main results, the predicted contours of particle concen-
own numerical implementation. Mortier et al.[84] performed tration at t ¼ 30 s after beginning of spraying are shown in
an extensive study on sensitivity analysis, calibration, intro- Fig. 6 (2D simulations) and Fig. 7 (3D calculations).
duction of a sub-model, and validation of the model by Generally, the outcomes of both 2D and 3D calculations
experiments on drying of wet pharmaceutical granules in a demonstrate that, for radial positions >0.1 m, the tempera-
fluidized bed at different drying temperatures. In all of the tures, predicted by the proposed model considering both
studied cases, good agreements between the calculated and droplet–droplet (DD) and particle–particle (PP) interac-
experimentally measured parameters (droplet=particle sur- tions, are higher, and the vapor mass fractions are lower,
face temperature, mass, and diameter) have been observed. compared to the corresponding data computed using the
16 MEZHERICHER ET AL.

over peripheral zones of the chamber. As a result, these


effects may reduce=increase an estimated particle fouling
on the dryer walls (compared to numerical simulations
considering droplet–droplet interactions only), which is
one of the main spray-drying operating problems.
In this way, the results of the performed study demon-
strate the importance of the introduction of particle–
particle collisions along with droplet–droplet into the mod-
eling of multiphase flow and transport phenomena in
spray-drying processes. The statistics on collisions obtained
in the numerical simulations of a spray-drying process indi-
cated that the frequencies of droplet–droplet and droplet–
particle (only ‘‘registered’’ but not treated in the performed
studies) interactions were comparable and substantially less
than the rate of particle–particle collisions in multiphase
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flow of the considered spray-drying set-up.

Case Study 2: Transport Phenomena in Spray-Drying


FIG. 6. Contours of particle concentration predicted by 2D
Process
axisymmetric model, t ¼ 30 s. (a) DDþPP model; (b) DD model;
(c) difference between the two models. (Reprinted with permission from To study heat and mass transport phenomena in
International Journal of Multiphase Flow, Vol. 43, Mezhericher, M.; Levy, spray-drying processes, the developed model of droplet
A.; Borde, I. Probabilistic hard-sphere model of binary particle–particle drying kinetics was enabled while the collision model was
interactions in multiphase flow of spray dryers, pp. 22–38, 2012, with off. The performed steady-state 2D and 3D numerical
permission from Elsevier.)
simulations have predicted patterns of air temperatures,
vapor fractions, velocities, droplet=particle trajectories,
model accounting for droplet–droplet interactions only. In evolution of droplet surface temperatures, droplet dia-
addition, the studies indicate that the total number of par- meters, droplet moisture contents, etc., in the adopted
ticles located inside the drying chamber were substantially spray-drying set-up. The outcomes of numerical studies
greater in the calculations using the DDþPP model than in have indicated important differences between the 2D and
the cases utilizing the built-in DD model in ANSYS FLU- 3D modeling. That is, the 3D simulations reveal
ENT software. At the same time, for cases when the three-dimensionality and asymmetry of the fields of tem-
DDþPP model was applied, the amount of small-size par- perature and vapor fraction in spray chamber, which coin-
ticles in the drying chamber was also larger compared to cides with other reports.[53,86] Moreover, it has been found
the calculations with the DD model. These substantial dif- that, compared to the 3D model, 2D simulations calculated
ferences in the amount of particles may be explained by the greater magnitudes of air velocity in the chamber center
shortcoming of the utilized ANSYS FLUENT code, which and lower air velocities at the periphery of the dryer. Such
in its original version coming from the software producer a difference can be explained by the intrinsic ability of the
has restricted capability of either treating all the 3D model to capture the transversal and asymmetric nature
inter-particle collisions as droplet–droplet ones (DD model of air and particle flows in the drying chamber, the feature
is turned on), or neglecting completely all the droplet– which 2D axisymmetric modeling is lacking. This con-
droplet and particle–particle collisions (DD model is clusion is supported by the results shown in Fig. 8, demon-
turned off). As a result, DD simulations accounted for strating the asymmetry of air flow field and the presence of
bounce and coalescence of all of the colliding droplet and the vortical transversal air flow predicted by the 3D model.
particle parcels as though it were droplet particles, while During the 3D numerical simulations, two different par-
the real nature of the colliding objects was not analyzed. ticle–wall boundary conditions were employed and exam-
From the outcomes of the numerical simulations, it fol- ined: particles ‘‘escape’’ from the simulations when
lows that, in contrast to the earlier published model of hitting the dryer walls and particles bounce back when par-
multiphase flow in spray dryers which accounted for ticle–wall collisions occur. However, if ‘‘particle rebound’’
droplet–droplet interactions only,[45,53] enabling the par- wall conditions were enabled, divergences of the numerical
ticle–particle collisions narrows and shifts the predicted solution have been obtained for 3D steady-state numerical
area of simultaneous heat and mass transfer between the simulations. This negative result may be attributed to an
continuous and dispersed phases towards the central region unsteady character of three-dimensional gas–droplet–
of the spray-drying chamber. At the same time, the particle flow promoted by the repeated recirculated motion
particle–particle collisions dissipate already dry particles of particles entrained in the air flow near the chamber
MULTI-SCALE MULTIPHASE MODELING 17
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FIG. 7. Contours of particle concentration predicted by 3D model, t ¼ 30 s. (a) DDþPP model; (b) DD model; (c) difference between the two models.
Left – XZ cut; middle – YZ cut; right – isometric view. (Reprinted with permission from International Journal of Multiphase Flow, Vol. 43, Mezhericher,
M.; Levy, A.; Borde, I. Probabilistic hard-sphere model of binary particle–particle interactions in multiphase flow of spray dryers, pp. 22–38, 2012, with
permission from Elsevier.)

walls: these particles repeatedly collide with walls, then capability of a comprehensive examination of gas and
bounce back into the flow and follow the air recirculation intra-droplet=particle transport phenomena, including
in the peripheral chamber regions. Such unsteady flow gas flow patterns, droplet=particle trajectories, and drying
characteristics of particles cannot be captured by the utilized kinetics. Figure 9 provides a detailed breakdown of par-
steady CFD solver,[47] and should be investigated separately ticle paths for different droplet initial diameters obtained
in further works involving unsteady simulations. in 3D steady-state numerical simulations (the droplet
One of the prominent benefits of CFD-based com- trajectories are shown individually for each injected drop-
putational simulations of spray-drying processes is the let diameter). The analysis of statistics of overall particle
18 MEZHERICHER ET AL.
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FIG. 8. Air velocity streamlines: (a) 2D axisymmteric simulations; (b)–(d) frontal, side, and isometric views, a 3D case study.[29]

residence times (PRTs, not presented here) and 3D great discrepancy is explained by the presence of lateral
particle trajectories (Fig. 9) leads to the conclusion that asymmetric air flows, which cannot be captured by the
droplets with initial diameters of 24.2 mm and 38.4 mm 2D axisymmetric modeling.[47]
have the longest PRTs and the lengthiest particle trajec- Figure 10 demonstrates the evolution of particle surface
tories in the spray dryer. These droplets have short relax- temperatures and the average moisture contents for
ation times and small Stokes numbers (less than 0.1), droplets predicted by 3D steady-state numerical simula-
which explain their multi-recirculating motion by air tions with the indicated initial diameters and trajectories.
entrainment occurring almost immediately after the As anticipated, the calculations show that larger droplets
atomization. Also, there is a considerable difference in have greater PRTs and longer duration of the first and
the averaged PRT predicted by the 3D and 2D second drying stages. Note that for the simulated spray-
spray-drying models: 3.9 s and 1.0 s, respectively; such a drying process the first drying stage takes substantially

FIG. 9. Three-dimensional particle trajectories for different spray droplets.[29]


MULTI-SCALE MULTIPHASE MODELING 19

between the dry particles and hot air is achieved rapidly


(see Fig. 10a), it can be concluded that for the last 75%
of their ‘‘chamber life,’’ silica particles are dry and have
temperatures which are close to those of the surrounding
drying agent. One may speculate that if ‘‘particle rebound’’
wall conditions would be utilized, the percentage of final
sensible heating period in PRT would be even greater.
It is worth noting that though Fig. 10 demonstrates the
behavior of selected droplet streams from the whole spray,
the rest of the injected streams exhibit similar trends, and thus
their description is omitted here for the space conservation.
In addition to the analysis of droplet streams, the
developed spray-drying model enables a detailed examin-
ation of drying kinetics of individual droplets. As an illus-
tration, curves of drying kinetics of a representative droplet
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with initial diameter 66.9 mm are given in Fig. 11a (the


droplet path is also shown in the figure). For detailed

FIG. 10. Simulated drying kinetics of spray droplets: (a) particle surface
temperatures; (b) particle moisture contents. The information is shown for
one stream of injected spray droplets. Initial diameters of the droplets and
droplet=particle trajectories are also indicated.[29]

longer compared to the second one, and their ratio is


roughly 3:1 for all particles. In addition, it is interesting that
the duration of the particle final sensible heating (calculated
here as the time from the end of the second drying stage and
until the particle either hits the chamber walls and
‘‘escapes’’ from the numerical simulations or leaves the
chamber through one of the outlets) has also been found
to be about three times greater than the overall droplet dry-
ing duration (including both drying stages). Therefore, the
performed numerical simulations have predicted the
approximate ratio of 3:1:12 between first, second, and final
sensible heating periods. In other words, for the simulated
spray-drying process, an average silica slurry droplet spends
19% of its residence time for the first drying stage (cf. to
one-third of the total dryer length, found by Woo et al.[87]
for 19.3 wt.% milk protein concentrate dried at 180 C in a
FIG. 11. Simulated drying kinetics of selected droplet (initial droplet
tall-form pilot-scale spray tower), just about 6% in the diameter 66.9 mm): (a) surface temperature and moisture content;
second drying stage, and in the remaining 75% of its PRT (b) temperature evolution of particle surface and center in the second
the heated particle is dry. Because a thermal equilibrium drying stage.[29]
20 MEZHERICHER ET AL.

analysis of the predicted drying kinetics, the interested Improving versatility—suitability for both types
reader is referred to the corresponding published study.[29] of droplets, containing either suspension or sol-
Another benefit from the developed model is its ability ution
to predict the evolution of temperature profile within Extensive validation by experiments on both
the wet particle of interest during the second drying stage, droplet and chamber scales, which require highly
as shown by Fig. 11b. One can establish that, for the accurate experimental measurements of droplet
average-sized droplet, the calculated maximum of intra- mass, size, and shape during drying; evolving tem-
particle temperature difference at the end of the second perature, pressure, and species distributions in
drying stage is equal to 1.1 C, which is close to the overall droplets=wet particles; parameters of droplet–
spray maximum of 1.4 C. These intra-particle temperature droplet, particle–particle, droplet–particle, and
differences, theoretically predicted even for such small droplet=particle–wall interactions; stickiness of
spray particles, are induced by intra-particle liquid evapor- wet particles and chamber fouling; unsteady
ation that cools the core of the wet particle in the second three-dimensional spray-gas turbulent mixing—
drying stage. The conclusion that intra-particle tempera- time-changing 3D patterns of gas pressure, velo-
ture differences are found even for micron-sized silica wet city, temperature, humidity, and droplet=particle
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particles is important, and indicates the presence of trajectories; and thermal and mechanical stresses
non-negligible, drying-induced internal thermal stresses. in the obtained product.
Consequently, these intra-particle stresses may potentially
lead to thermal damage of the obtained final product.[35,36]
NOMENCLATURE
a empirical coefficient
CONCLUSIONS
A surface area, m2
This article summarizes the results of modeling of
b empirical coefficient; offset between two
transport phenomena in a spray-drying process performed
droplet centers, m
by our research group during the last several years. The
B Spalding number
spray-drying model utilizes a multi-scale multiphase
Bi Biot number
approach: the advanced model of single droplet drying
c empirical coefficient; mass concentration
kinetics is coupled to a Eulerian–Lagrangian description
of solid fraction, kg  kg1
of gas-spray mixing and the overall formulation is solved
cp specific heat under constant pressure,
numerically using a CFD technique. The model has been
Jkg1 K1
successfully validated and utilized for prediction of drying
d droplet=wet particle diameter, m
behavior of single droplets of suspensions=solutions, and
dc diameter of crust capillary, m
two- and three-dimensional steady-state calculations of
dp diameter of primary solid particles;
spray-drying processes.
droplet=particle diameter, m
More generally, theoretical modeling and numerical
Dv coefficient of vapor diffusion, m2 s1
simulations of spray-drying processes are active areas.
e coefficient of normal restitution
Studies of spray drying published during the last few years
E Young’s modulus, Pa
demonstrate substantial scientific progress in the realistic
Es,0 Young’s modulus of solid component, Pa
description of the associated multiphase flow and
DEv apparent activation energy, Jmol1
multi-scale transport phenomena. This advancement
F force, N
provides engineers with more accurate, high-quality tools
FA virtual mass force, N
for innovative design of spray-dryer systems and for choos-
FB buoyancy force, N
ing suitable operating conditions, enabling engineering of
FC contact force, N
particles with desired properties.
FD drag force, N
Expected new developments for computational models
FGP pressure gradient force, N
of spray drying are the following:
Fo Fourier number
Enabling prediction of morphology and micro- g gravity acceleration, m  s2
structure of obtained product h heat transfer coefficient, Wm2 K1;
Accounting for both unsteady and three- specific enthalpy, Jkg1
dimensional nature of spray-drying processes hD mass transfer coefficient, m  s1
Accounting for droplet–droplet, droplet–particle, hfg specific heat of evaporation, J kg1
particle–particle, droplet–wall, and particle–wall k thermal conductivity, Wm1 K1;
interactions along with realistic droplet drying turbulent kinetic energy, m2s2
kinetics Kn Knudsen number
MULTI-SCALE MULTIPHASE MODELING 21

m mass, kg; number of collisions that k molecular mean free path, m


collector undergoes l dynamic viscosity, kg  m1  s1;
_v
m mass transfer rate, kg  s1 coefficient of dynamic friction
M molecular weight, kg  mol1 n Poisson’s ratio; kinematic viscosity, m2s1
n empirical coefficient; spread parameter; q density, kg  m3; density of gas
number of droplets=particles phase, kg  m3

n mean expected number of collisions r mechanical stress, Pa
nparcels number of parcels [rt] particle tensile strength, Pa
nparticles number of droplets=particles rT thermal stress, Pa
Nu Nusselt number s duration, s; dimensionless time of
p pressure, Pa particle drying; shear stress, Pa
P probability distribution t velocity, m  s1
P1 probability of at least one collision u relative humidity
Pr Prandtl number w fractionality coefficient
specific heat of mixing, Jkg1
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qt xv vapor fraction
r radial space coordinate, m
Subscripts
R radius, m
Rm random number between 0 and 1 a air, dry air fraction
< universal gas constant, Jmol1 K1 atm atmospheric
Re Reynolds number c crust capillary; collision
s space coordinate, m cr particle crust; critical
Sc Schmidt number d droplet
Sh Sherwood number f final point of drying process
t time, s g drying agent; gas phase
T temperature, K i crust-wet core interface
Tm temperature of melting point, K in inflow
u velocity of drying agent, m  s1 ip initial heating-up period
~p
U vector of particle velocity, m  s1 m air-vapor mixture
u
~ vector of gas velocity, m  s1; vector of max maximal
collector=contributor velocity, m  s1 min minimal
ur relative velocity between collector and new new
contributor, m  s1 out outflow
V volume, m3; cell volume, m3 p droplet=particle
We Weber number pores crust pores
x space coordinate, m; level from chamber r radial direction
top for 2D simulations, m s solid fraction; surface
X moisture content (dry basis), kg  kg1 sat saturation
y space coordinate, m tot total
z space coordinate, m; level from chamber v vapor; vapor fraction
top for 3D simulations, m w water
Greek letters wc particle wet core
a thermal diffusivity, m2s1 z axial direction
am empirical coefficient 0 initial point of drying process
aT coefficient of thermal expansion, K1 1 starting point of droplet evaporation
b empirical coefficient period; collector
b0 coefficient of tangential restitution 2 contributor
c ratio of specific heats 1 bulk of drying agent
d droplet void fraction h tangential direction
Dt calculation time step, s
e crust porosity; dissipation rate of
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