Drying Technology

An International Journal

ISSN: 0737-3937 (Print) 1532-2300 (Online) Journal homepage: http://www.tandfonline.com/loi/ldrt20

Theoretical Models of Single Droplet Drying

Kinetics: A Review

M. Mezhericher , A. Levy & I. Borde

To cite this article: M. Mezhericher , A. Levy & I. Borde (2010) Theoretical Models
of Single Droplet Drying Kinetics: A Review, Drying Technology, 28:2, 278-293, DOI:
10.1080/07373930903530337

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 Drying Technology, 28: 278293, 2010
Copyright # 2010 Taylor & Francis Group, LLC
ISSN: 0737-3937 print=1532-2300 online
DOI: 10.1080/07373930903530337

Theoretical Models of Single Droplet Drying Kinetics:

A Review
M. Mezhericher, A. Levy, and I. Borde
Pearlstone Centre for Aeronautical Engineering Studies, Department of Mechanical Engineering,
Ben-Gurion University of the Negev, Beer-Sheva, Israel

resistance to mass transfer because of the crust layer. The

During the last decades, growing attention has been given to second drying stage continues until the particle moisture
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theoretical and experimental studies of drying behavior of single
droplet containing solids. This research interest is motivated by
the need for fundamental understanding of the drying phenomena
in extensively used technological processes like spray drying, ui-
dized bed drying, pneumatic drying, etc., at drop-wise and particu-
late levels. The present literature review summarizes the developed
theoretical models of single droplet drying kinetics, discovers their
benets and deciencies, and identies prospects for future research.
Keywords Droplet; Drying kinetics; Modeling; Particle
INTRODUCTION
Formation technologies like spray drying, uidized bed
drying, freeze drying, pneumatic drying, solution aerosol
thermolysis, etc., involving drying of droplets containing
small solid particles are utilized today in many industries,
among them are food and dairy manufacturers, chemical
and biochemical industries, pharmaceutical and ceramics
production, and others.[1,2] The theoretical models of such
processes are based on description of drying kinetics of
individual droplets, which turn into wet and then dry
particles during the drying process.
The drying kinetics of droplets containing solid compo-
nents is usually divided in two drying stages. In the rst
drying stage, the droplet with excess of liquid is subjected
to the ow of drying gas (air, steam, nitrogen, etc.), gains
sensible heat, and begins to evaporate from the surface.
This liquid evaporation results in droplet diameter shrink-
ing and simultaneous increase of solids concentration near
the droplet surface. The latter leads to the precipitation of
solid fraction at the droplet surface and, eventually, the
surface becomes covered with a layer of solid component
called crust.[3] At this moment, the droplet turns into a
wet particle and the second drying stage commences. In
this stage, the drying process is hindered by additional
Correspondence: A. Levy, Pearlstone Centre for Aeronautical
Engineering Studies, Department of Mechanical Engineering,
Ben-Gurion University of the Negev, P.O. Box 653, Beer-Sheva
84105, Israel; E-mail: avi@bgu.ac.il
content reduces to equilibrium value with the drying
medium. After that the drying process actually stops and
the particle is heated up to the equilibrium temperature.
Typical droplet temperature and moisture content evolu-
tions during drying process are shown in Fig. 1. In this
gure, the interval between points 0 and 1 is corresponding
to the droplet initial heating, the period between points 1
and 2 is related to the droplet evaporation period, the inter-
val between points 2 and 3 to the second drying stage, and,
nally, the period between points 3 and 4 designates the
particle heating up to equilibrium with the surrounding
drying agent.
The published theoretical models of droplet drying
kinetics can be related to the following categories: models
based on a semi-empirical approach that utilizes the concept
of characteristic drying curve (CDC);[47] deterministic dry-
ing models, which describe the processes within the droplet
using the continuity, momentum, energy, and species con-
servation equations;[5,819] recently appeared deterministic
models with distribution of solid component described by
population balance;[2023] and novel drying models based
on reaction engineering approach (REA).[2428] Each
category of droplet drying models has its benets as well
as drawbacks briey discussed below.
The semi-empirical CDC models of droplet drying
kinetics are usually represented by a small set of simplied
equations allowing fast computations and are known to
work well for small particle sizes.[29] In such models, the
rst drying stage is simplied by analogy with evaporation
of small pure liquid droplet. For the falling rate period, the
drying rate in a CDC model is determined by the drying
rate at the end of the rst drying stage multiplied by a
function depending on critical, equilibrium, and current
moisture content values. The functional form of the above
dependency and the critical moisture content are tted to
an experimental drying curve. Moreover, the value of criti-
cal moisture is taken as a constant for the specic material.
According to Fyhr and Kemp,[6] the theoretical simplicity
of CDC models is disbursed by their shortcomings; among

278
 MODELS OF SINGLE DROPLET DRYING KINETICS
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FIG. 1. Typical drying evolutions of droplet temperature (a) and
moisture content (b). D0: initial diameter, Dp: particle diameter, Di:
internal diameter, X0: initial moisture content, Xcr: critical moisture
content, and Xe: equilibrium moisture content.
them is poor model suitability for the drying conditions dif-
ferent from those originally used in the model development.
The deterministic analytical models of single droplet dry-
ing describe the process by a set of differential equations
with corresponding initial and boundary conditions. The
solution of this set of equations is complicated by the
presence of a moving domain boundary because of
the shrinking droplet radius in the rst drying stage and
the receding interface between the dry crust and wet core
regions of the wet particle in the second drying stage.[17,30]
As a result, the numerical solution of such models is a
complex problem and the simulation of the drying process
can demand signicant computer resources and time. In
addition to the effortful numerical solutions, deterministic
models usually require knowledge of many coefcients like
thermal and mass diffusivities, particle porosity, critical
moisture content, etc., under different moisture and
temperature conditions. The appropriate values of the men-
tioned coefcients often cannot be found in the published
279
sources and thus require either conducting experimental
measurements or usage of questionable tting techniques.
Nevertheless, the behavior of the main drying characteris-
tics can be predicted for various drying conditions showing
a good accuracy and consistency with experimental data,
and this opens up possibilities for both fundamental and
applied studies of single droplet drying by utilizing such
analytical models.
The REA models, which have appeared in recent years,
demonstrate a ne agreement with experiments as well as
fast calculations and reduced demands of the computer
resources. However, at the present time the application of
REA for droplet drying kinetics is still limited by the range
of materials whose drying behavior was already exper-
imentally studied. The reason is that the REA approach
utilizes an empirical correlation connecting between the
partial vapor density over the droplet surface and the aver-
age droplet moisture content. This empirical correlation
should be determined experimentally for each material
whose drying behavior is modeled at different moistures.[31]
It is worth noting that such feature of REA is similar to
necessity of functional tting to experimental drying curve
in a CDC approach. For detailed comparison between
CDC and REA models and their predictions, the reader
is referred to the studies of Chen and Lin[24] and Patel
and Chen.[32] Nevertheless, the REA-type models and
applications of the REA approach in combination with
analytical drying kinetics models[17,18] are undoubtedly
promising due to their simplicity and high accuracy at dif-
ferent drying conditions.
From the point of view of their application, the pub-
lished theoretical models of single droplet drying kinetics
are usually suitable only for droplets containing insoluble
solids (slurries or suspensions) or solely for droplets with
dissolved solids (solutions). Some of the models are more
versatile and can be implemented for both types of droplets
as well as for droplets containing concurrently dissolved
and insoluble solids. Such classication of the models in
three main groups depending on their ability to deal with
specic droplet type has advantages of simplicity and prac-
tical orientation. In turn, each of these three model families
can be subdivided into categories of CDC, deterministic,
population balance, and REA-based models mentioned
above. Using this classication, the following sections rep-
resent a detailed overview of the published models of single
droplet drying kinetics.
DRYING KINETICS MODELS OF SINGLE DROPLET
CONTAINING INSOLUBLE SOLIDS
Published Models
One of the rst drying kinetics models suitable for dro-
plets with insoluble solids was a receding interface drying
model for slurry droplet of sodium sulphate decahydrate
 280 MEZHERICHER ET AL.
proposed by Cheong et al.[33] It was a two-stage drying
kinetics model where in the rst drying stage, a uniform
droplet temperature was assumed during initial period of
droplet heating and subsequent period of equilibrium evap-
oration. In the second drying stage, the density of particle
wet core was taken as a constant value and its temperature
distribution was neglected. The temperature and vapor
concentration proles in the particle crust were unjusti-
ably assumed to be linear. In addition, the crust heat
capacity was considered to be insignicant. As a result,
the authors reported a strong discrepancy between the pre-
dicted and measured droplet temperatures, especially in the
second drying stage. This discrepancy was explained by an
arguable hypothesis: the measured temperature was that of
the particle crust, whereas the model predicted the actual
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temperature of the particle wet core.
A theoretical drying model based on Stefan-type vapor
diffusion in the second drying stage was developed by
Abuaf and Staub.[9] The period of initial droplet heating
was neglected. In the second drying stage, the vapor ux
for a single straight crust capillary was found from the
Stefan-type steady-state diffusion equation and the vapor
diffusion coefcient was considered as independent of tem-
perature. The drying rate of wet particle was determined by
multiplying the vapor ux by the cross-sectional area of all
the capillaries and the void fraction of the crust. It must be
noted that such an assumption is not fully consistent,
because the void fraction is a volumetric ratio, whereas
the ux must be multiplied by the area surface ratio
between the pores and the crust. In addition, the tempera-
ture prole in the particle wet core and the crust heat
capacity were neglected by the authors. At the same time,
the temperature difference between the particle surface
and its center was evaluated. Unfortunately, though the
model was tested by simulating the drying behavior of coal
slurry droplets, the results of the model validation were not
presented by the authors.
In the theoretical study of Borde and Zlotnitsky[13] they
proposed treating the droplet with insoluble solids as a
pseudo-porous body. Thus, the droplet void fraction in
both drying stages was determined with the help of
parameter called the transient porosity coefcient, which
allowed authors to describe the droplet drying without sep-
arate modeling of the rst and second drying stages. The
droplet drying rate was calculated with the help of
expression analogous to that developed by Abuaf and
Staub[9] but simplied using the assumption that partial
vapor pressure in the particle crust was small when com-
pared to the total ambient pressure. However, the above
assumption is valid for relatively low temperatures of the
drying agent. The authors also neglected the temperature
differences in the particle wet core but considered the ther-
mal inequality between the particle surface and its center. It
is worth noting that unlike the study of Abuaf and Staub,[9]
the vapor diffusion coefcient was treated as temperature
dependent and the crust heat capacity was considered in
the model. The authors did not cite the results of the model
validation though the theoretical study of coal slurry
droplets drying was performed.
The single droplet drying model published by Abuaf and
Staub[9] was extended later on by Levi-Hevroni et al.[14] A
steady-state parallel ow of slurry droplets in hot atmos-
pheric air was considered. The air temperature was chan-
ging along the drying chamber. The authors proposed
evaluating the crust thermal conductivity with the help of
correlation that took into account its spherical geometry.
The other model equations were analogous to those pre-
sented in Abuaf and Staubs[9] study. However, the results
of the model validation were not reported.
In the mathematical model developed by Elperin and
Krasovitov,[15] the solid-to-liquid volume ratio was utilized
as a droplet drying characteristic instead of traditional
droplet moisture content (liquid-to-solid mass ratio). The
period of initial heating of the droplet was not considered.
The rst drying stage was described by the set of mass and
energy conservation steady-state partial differential
equations (PDEs) only for drying ambient, so the tempera-
ture gradient inside the droplet was neglected. The PDE set
was solved analytically assuming that the properties of
boundary layer around the droplet were independent of
the droplet surface temperature. In the second drying stage,
the temperature prole in the particle wet core was
neglected, and the set of mass and energy conservation
PDEs was developed only for crust region and drying
ambient under steady-state conditions. This set of PDEs
was reduced to the set of algebraic equations by assuming
that coefcient of vapor diffusion and thermal conductiv-
ities of the drying agent and porous crust were temperature
independent. The drying rate of a wet particle was calcu-
lated with the help of an equation developed by Abuaf
and Staub.[9] The validation results of the model, tested
by simulation of coal-water slurry droplet drying, were
not published.
Minoshima et al.[34] developed a simplied granulation
model of a single droplet by considering only the rst dry-
ing stage. It was assumed that after the rst drying stage
the particle outer diameter did not change and the droplet
turned into a hollow particle with a central void. The
authors investigated several factors that affect the diameter
and strength of the nal particle (granule). It was assumed
that the primary particles inside the droplet were motion-
less and were held on the droplet surface by surface tension
during the droplet shrinkage. The diameter of the granule
was determined by the balance condition between the par-
ticle strength and the external compressive pressure exerted
by ltration under the drying conditions and the drying
process. Analyzing the simulation results obtained for
silica slurry drying, it was concluded that the granule
 MODELS OF SINGLE DROPLET DRYING KINETICS
diameter, crust thickness, and particle strength increased
with increasing initial solid concentration of the silica
slurry and initial droplet diameter. At the same time, the
size of particle central void showed non-multiple-valued
dependency on the initial solid fraction and demonstrated
tendency to increase with the droplet diameter. Minoshima
et al.[35] experimentally veried the developed model by
comparing the predicted granule diameters with those
obtained from granulation experiments of aqueous silica
slurry drying. In these experimental studies, the dried dro-
plets contained 0.3 mm primary particles suspended in
water without any binder and were dispersed by means
of a spinning disk. In general, the experimental results con-
rmed the above-mentioned theoretical predictions regard-
ing the dependency of the nal particle diameter on the
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initial solid fraction and droplet diameter.
A theoretical description of the rst stage of single
droplet drying in an ultrasonic eld was presented by Yarin
et al.[36] The model is suitable for droplets containing
suspended particles and was experimentally validated by
drying of water droplets with 30-mm glass beads in an
acoustic tube levitator. The theory predicted the evolution
of droplet radius and droplet drying rate by taking into
account the convective term of the acoustic streaming on
the mass transfer from the droplet.[37] Further, a uniform
droplet temperature was determined from the thermal bal-
ance associated with the evaporation=condensation
processes and heat removal from the droplet surface. Both
calculations and experimental measurements demonstrated
the decrease of the droplet size due to evaporation, the
droplet rise in the acoustic eld as its mass decreased,
and droplet shape evolution during drying. It was found
that at a certain moment the continuous droplet size
reduction ceased and afterwards the droplet diameter
remained constant, which was attributed to the crust
formation. Variation of drying parameters like air tem-
perature in the range 2384 C, initial solid mass fraction
between 0.050.3, and droplet volume among 0.26
1.02 mL showed good agreement between the predictions
and experiment as well. Though the work did not propose
any theoretical formulation for the second drying stage,
some physical estimates were given; e.g., the authors[36]
explained the reason of the crust precipitation observed
at the beginning of the rst drying stage. It was suggested
that the acoustic radiation pressure at the top and bottom
of the droplet can lead to formation of particleparticle
contacts between the primary particles of the outer crust
layer. This in turn results in additional adhesive pressure
due to London-van der Waals forces acting through such
contacts. The adhesive pressure leads to the occurrence of
a percolating cluster that pushes the liquid toward the
equatorial droplet area and as a result, the ratio between
the equatorial and meridional radii (called also aspect
ratio) suddenly increases. In addition, the authors argued
281
that the pure diffusion-driven evaporation in the crust
pores is much slower than the acoustically driven evapor-
ation from the particle surface and thus the vapor diffusion
in the pores is a limiting process in the second drying stage.
Discussion
As it follows from the literature survey, most of the
published drying models of droplets containing insoluble
solids treat the rst drying stage as though the droplet is
composed only of the liquid fraction, disregarding the
process of diffusion and agglomeration of the suspended
primary particles. As a result, the transition point, in which
a thin layer of crust is formed at the outer droplet surface
and the droplet turns into wet particle, is not calculated
rigorously analytically but is derived from a certain critical
average solid-to-liquid ratio. This ratio is usually considered
as a predened constant value for the given material. How-
ever, the studies performed by Liang et al.[38] for the rst
drying stage of silica slurry droplet showed that the point
of crust formation (and therefore, critical solid-to-liquid
ratio) varies depending on the drying medium temperature,
humidity, velocity, droplet initial moisture content, size of
primary particles, etc. The simplications made in the most
of the published drying models of single droplets with inso-
luble solids do not allow calculations of primary particles
distribution within the droplet=wet particle and, conse-
quently, the structure and morphology of the nal product
can not be adequately theoretically predicted. Further, in
spite of the unsteady character of heat and mass transfer
during the drying process of droplet containing solids, the
rate of moisture transfer from the droplet is usually determ-
ined using a simplied steady-state assumption. To the best
of our knowledge, except for Minoshimas group,[34,35,38]
the other researchers did not investigate the reasons leading
to formation of particles with different nal structures, such
as solid dense particles and hollow particles with a void
obtained in the real drying processes of the droplets con-
taining insoluble solids.
Another important aspect is the contradicting assump-
tion of uniform droplet temperature in most of the pub-
lished drying models of droplet containing insoluble
solids. As a rule, this presumption is justied by estimated
value of Biot number <0.1. However, for unsteady pro-
cesses both conditions of Bi <0.1 and Fo >0.1 must be
satised to vindicate the temperature uniformity.[39] More-
over, because of the thickening particle crust in the second
drying stage, the classical formulation of Biot and Fourier
numbers is inadequate for the droplet drying kinetics. The
case of uniform temperature distribution was discussed
with special attention in the studies by Chen,[40] Patel
et al.,[41] and Patel and Chen[27] where the drying of food
droplets with dissolved solids was considered. In the above
papers the authors proved that for drying air temperatures
up to about 150 C temperature differences in the solution
 282 MEZHERICHER ET AL.
droplet were negligible. At the same time, in the reports of
Mezhericher et al.[1719,42] for silica slurry droplets (which
will be discussed in following sections), a uniform droplet
temperature was observed in the rst drying stage, whereas
in the second drying stage, due to the crust formation and
thickening, the particle temperature distribution was
predicted to be close to the uniform distribution only for
the temperatures of drying air below about 150 C, and
for higher drying temperatures up to 750 C the tempera-
ture difference between the particle surface and its center
was already signicant. It is worth noting that these
temperature differences and corresponding thermal stresses
within a small wet particle can be lead to product degra-
dation and damage observed in the real drying processes
under elevated temperatures.[18,42] Therefore, in general,
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for droplets containing insoluble solids the internal tem-
perature distribution can be neglected in the rst drying
stage and have to be considered in the second stage of
drying, especially for the cases with high temperature of
the drying agent.
DRYING KINETICS MODELS OF SINGLE DROPLET
CONTAINING DISSOLVED SOLIDS
Published Models
One of early known attempts to devise the deterministic
model suitable for droplets with dissolved solids was
accomplished by Marshall.[43] The model equations were
based on pure liquid droplet evaporation theory with the
correction accounting for decrease of the vapor pressure
and droplet temperature increase due to presence of solids
in the solution. The developed model was capable of calcu-
lating the droplet surface temperature and drying rate in
quiescent and moving drying air. The effect of curvature
on vapor pressure increase was taken into account and it
was shown that this increase remained smaller than 1% for
droplet diameters larger than 0.2 mm. The problem of evap-
oration at high air temperatures was outlined by consider-
ing sensible heat transferred to the gas lm surrounding the
evaporating droplet. However, the falling rate period of
droplet drying was described only qualitatively and a com-
plete set of equations for this stage was not developed.
Charlesworth and Marshall[3] studied the evaporation
from single aqueous droplets containing dissolved solids
of sodium sulphate, potassium sulphate, copper sulphate,
ammonium nitrate, calcium chloride, sodium acetate,
lithium hypochlorite, sucrose, blue dye, polyvinyl acetate
resin, whole fresh milk, and coffee extract. In part I of
their report, Charlesworth and Marshall[3] proposed a
theory of single droplet drying kinetics based on
assumptions of spherical symmetry, absence of internal
circulation, diffusion-driven mass transfer within the
droplet, and constant droplet diameter. Such simplica-
tions allowed derivation of an analytical representation
of time-dependent concentration proles within the dried
droplet and prediction of crust formation moment. The lat-
ter equation was later corrected using the results of
experimental studies performed on different single droplets
suspended in air ow. It is noted that the authors did not
suggest any theoretical correlation for droplet temperature.
Furthermore, the results of the predicted concentration
proles within the droplet were not presented in the report.
The unsteady character of droplet drying was con-
sidered in the semi-empirical model developed by Furuta
et al.[44] The main purpose of Furutas model was to use
it in the modeling of the spray-drying processes of food
droplets. In this model, the concentration prole of droplet
moisture was described by partial differential equations of
species conservation in both drying stages. Further, a
uniform droplet temperature was determined by the heat
balance equation involving droplet heat capacity changing
during drying. In addition, experimental measurements
were proposed as a method for determining the vapor mass
transfer rate during the wet particle drying. No validation
results of the proposed model upon single droplet drying
were reported.
The period of initial droplet heating was ignored and the
droplet moisture content was connected to experimentally
obtained droplet evaporation rate in the semi-empirical
model of single droplet drying developed by Kuts et al.[5]
The droplet=particle temperature was assumed to be
uniform and Luikovs experimental correlation between
dimensionless particle temperature and moisture evapo-
ration rate was utilized. The heat capacity of the particle
crust was neglected. The predicted droplet=particle
temperatures were reported to be in deviation of 1015%
from experimentally obtained for liquid substrate of
entobacterin.
A simplied drying kinetics model developed by
Dolinsky[16] can be utilized for rapid but rough estimation
of the droplet drying duration. By neglecting the period of
initial droplet heating, the author proposed an analytical
expression for uniform droplet temperature calculation in
the rst drying stage. In the second stage, the crust
temperature prole was arguably assumed to be linear,
the wet core temperature was supposed to be uniform,
and the particle surface temperature was calculated from
a simplied expression based on the steady-state assump-
tion. In addition, the particle drying rate in the second
stage was calculated using the supposition that the particle
mass decreased with a constant rate. Time-dependent drop-
let moisture content was treated as uniform in both drying
stages. No validation of the model was presented.
An analytical model of single droplet drying was
presented by Kuts et al.[5] in the same article in which the
authors proposed the semi-empirical model discussed
above. The crust heat capacity was taken into account. It
was suggested that average droplet=particle moisture
 MODELS OF SINGLE DROPLET DRYING KINETICS
content can be either a linear or exponential function of the
drying time. In the rst drying stage, the droplet
temperature was assumed to be uniform and the period
of initial droplet heating was disregarded. In the second
stage, the temperature proles in the crust and wet core
regions were described by appropriate set of PDE equa-
tions of energy and mass conservation. However, an argu-
able boundary condition was utilized in the equations set:
the temperature of the crustwet core interface was
assumed to be constant and equal to the wet bulb tempera-
ture of drying air. It should be noted that according to the
experimental studies performed by Cheong et al.[33] and Ali
et al.,[45] the temperature of the crustwet core interface is
time dependent and increases considerably over the wet
bulb value during the second drying stage. Based on the
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assumption of uniform temperature distribution in the
region of particle wet core, Kuts et al.[5] have obtained
several analytical expressions: the temperature inside the
particle crust as a function of time and radial coordinate
and time-dependence of position of the crustwet core
interface during drying. The authors developed two expres-
sions for calculation of the drying process duration,
depending on the assumption of moisture content behavior
(linear or exponential). The performed theoretical calcula-
tions of estimated drying process duration showed up to
15% discrepancy from the performed experimental
measurements in two case studies of entobacterin substrate
droplet drying.
Sano and Keey[8] developed a theoretical model that
calculated the prole of moisture concentration inside the
dried droplet and wet particle with a central void. The
moisture distribution was described using a species balance
PDE accounting for diffusion and internal circulation and
corresponding boundary conditions. The droplet tempera-
ture was assumed to be uniform in both stages of drying.
Further, the effect of possible wet particle ination and
rupture during drying was taken into account. Experimen-
tal investigations included the studies of skim milk droplet
behavior during drying in atmospheric air under different
conditions. The agreement between the predicted and mea-
sured data of skim milk drying kinetics was found to be sat-
isfactory. However, the comparison between the model
predictions and experimental data provided by Trommelen
and Crosby[46] showed a substantial discrepancy, and this
inconsistency was not properly explained by the authors.
Hecht and King[47] proposed two models for prediction
of particle morphology and retention of volatile substances
during drying of droplet with dissolved solids. The rst was
a simple model predicting the drying rate and temperature
history of a 30% sucrose droplet during the period of mor-
phological development when the droplet temperature was
above boiling point. The model assumed that the droplet
drying rate was controlled by the rate of heat transfer from
the drying gas and neglected the energy accumulation by
283
the droplet. To match the experimental data, the authors
utilized a tting parameter accounting for the heat added
by conduction to the droplet from the solid support, the
increased surface area, and the effect of droplet ination.
The second numerical model involved the convective
diffusion equations for a droplet containing SF6, water,
and sucrose. To simulate the effects of morphological
development, a concept of single and never rupturing
central bubble containing water vapor, SF6, and inert gas
was incorporated. Droplet temperature was assumed to
be a uniform and concentration proles in the liquid were
treated as radially symmetric. The model was successfully
validated by comparison of the predicted and experimental
droplet drying rates and SF6 loss rates (for details of
experimental setup see Hecht and King[48]). However, the
validation of the predicted particle temperature was not
presented. The calculations also demonstrated the reten-
tion of SF6 during drying without internal bubble rupture
and this was conrmed by experimental observations as
well. On this basis, the authors suggested that if the liquid
inside drops in a spray dryer could be mixed without the
bursting of bubbles, then the drying rate might be
enhanced without losses of volatile components.
Frey and King[49] developed a mathematical model of
droplet drying in the constant rate period. The model is
suitable for a foam-spray-drying process that is a modi-
cation of a conventional spray-drying process including
articially introduced bubbles into the spray droplets;
sometimes this process is also called aeration; see Walton
and Mumford.[50] The authors focused their attention on
the constant rate drying period because of its particular
importance in the studies of aroma retention: according
to Thijssen and Rulkens[51] and Menting,[52] the majority
of aroma loss from droplets takes place during this period.
Unlike previous models of foamed droplets drying, which
either considered droplets containing a single, centrally
located bubble[8,53] or droplets of constant radius[54] Frey
and King[49] described the behavior of a shrinking droplet
with multiple internal bubbles. Despite this, the model pre-
dictions were found to be relatively insensitive to assump-
tions concerning the form of the dispersed gas in the
droplet. Particularly, calculations assuming a single, large,
centrally located internal bubble were similar to simulation
results presuming that the same amount of gas is dispersed
in a number of small bubbles that move with the velocity of
the nonvolatile solute. The simulations also indicated that
the diffusion losses of volatiles (aroma) were increased
when bubbles were introduced into the droplets. This
mathematical analysis for foamed droplets, adopted subse-
quently by Wallack et al.,[55] was afterwards conrmed by
experimental measurements by Frey and King.[56]
A theoretical model of single droplet drying capable of
temperature and moisture proles prediction was
developed by Sloth et al.[57] The authors, similarly to
 284 MEZHERICHER ET AL.
Wijlhuizen et al.[53] and Sano and Keey,[8] regarded the
drying process as continuous without separate formulation
of drying stages. However, in contrast to Wijlhuizen
et al.[53] and Sano and Keey,[8] the authors argued that
the drying kinetics model suitable for many different drop-
let compositions and sizes over a broad range of drying
conditions must include the calculation of droplet tempera-
ture prole. It was assumed that the drying process resulted
in solid and dense nal particles without voids. Neglecting
internal circulation and presuming ideal solution, Ficks
law of diffusion was utilized to describe the mass transfer
rate inside the droplet. Further, the droplet temperature
prole was formulated by energy conservation PDE. To
provide the model validation, droplets of aqueous solu-
tions of maltodextrin and trehalose were dried in an ultra-
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sonic levitator at low air temperatures in the range of
2760 C. The water diffusivity in the above solutions was
calculated as a function of water fraction and independent
of temperature. The inuence of acoustic streaming was
taken into account by calibration of the model with experi-
mental drying kinetics of pure water droplets. The results
of comparison between the predicted and measured droplet
radii showed a good agreement in all studied cases of mal-
todextrin and trehalose solutions drying. At the same time,
the calculated evolutions of the droplet temperature and
water fraction were not validated by any experimental
data. The presented proles of the water fraction indicate
that at a certain moment the water fraction decreases to
zero at the droplet outer surface. This corresponds to dry
skin initial formation (which is typical for organic materi-
als; see Walton and Mumford[58]) and transformation of
droplet into a particle. However, instead of subsequent
skin thickening inward as it would be expected[58] and cor-
responding propagation of points of zero water fraction
toward the droplet center to form a solid particle, the
model demonstrates a gradual reduction of the water frac-
tion prole as drying proceeds, whereas zero water fraction
is established only at the droplet surface. In addition, the
reported results lacked the comparison between the predic-
ted and experimental history of droplet mass.
A one-dimensional model of single droplet drying based
on the assumption of Ficks diffusion mass transport inside
the droplet was proposed by Brenn et al.[59] Internal macro-
scopic ow and circulation were disregarded. The descrip-
tion of the Sherwood number for evaporating solvent was
performed using the model of Abramzon and Sirignano.[60]
The second drying stage was not modeled. The derived
PDE of liquid concentration elds inside the droplet was
rendered to nondimensional form and a characteristic
parameter representing the inverse of the Sherwood num-
ber was indicated. It was postulated that this parameter
can be a characteristic morphological parameter separating
the drying regimes with formation of hollow and solid
nal particles. Further, the authors utilized Fords[61]
experimental data for drying of droplets containing water
solution of sodium chloride. Using this information, the
threshold value of the characteristic parameter was esti-
mated to be 3.3. To verify their hypothesis, a set of mea-
surements of sodium chloride droplet drying in an
acoustic levitator was conducted. In these experiments,
the initial salt mass fraction was varied between 4 and
18% and the drying temperature was in the range of
1070 C, resulting in the characteristic parameter between
2 and 12.6. In addition, several experimental runs were car-
ried out in a spray dryer of Degussa AG. All the experi-
mental observations conrmed that the drying conditions
with the characteristic parameter <3.3 led to formation
of hollow nal particles and for the values of the character-
istic parameter >3.3 solid nal particles were obtained,
thereby validating it as a characteristic morphological
parameter. The authors proposed future work to determine
the values of the characteristic morphological parameter
for other substances and to extend their approach on sus-
pensions as well.
Adhikari et al.[62,63] extended the modeling approach
proposed by van der Lijn et al.[64] to sticky food droplets
and accounted for a glass transition temperature. Time-
dependent proles of moisture content and uniform tem-
perature in non-hollow spherical droplet were calculated
using the mass diffusion PDE and lumped heat capacity
energy balance equation for both drying stages. Unfortu-
nately, the authors proposed a boundary condition at the
outer droplet surface that supposed that the vapor ux
leaving the droplet surface emerged solely due to internal
diffusion transport of liquid and disregarded the term
corresponding to the shrinkage of the droplet surface. In
contrast, such term was taken into account by Sano and
Keey,[8] Brenn et al.,[59] and Yarin et al.[65] Nevertheless,
the results of the numerical simulations demonstrated a
reasonable agreement with the experimental mass, tem-
perature, and surface stickiness measurements of fructose
and lactose droplets dried at 65 and 80 C.
A theoretical drying model of skim milk and whole
milk single droplets, based on the REA approach, was
developed by Chen and Lin.[24] A uniform droplet tempera-
ture was assumed. The mass transfer rate was determined
as a function of the difference between the vapor concen-
tration values at the droplet=wet particle liquid interface
and in the bulk of drying medium. The vapor concen-
tration at the interface was connected to its saturation
value with the help of a fractionality coefcient. In turn,
this fractionality coefcient was expressed by an Arrhenius
equation using apparent activation energy (AAE) and
droplet temperature. The values of AAE for skim and
whole milk single droplets were found experimentally as
functions of two parameters: (a) the difference between
the average moisture contents of droplet and bulk air
and (b) the AAE value of the drying air. In addition, the
 MODELS OF SINGLE DROPLET DRYING KINETICS
droplet=particle uniform temperature was described by an
ordinary differential equation of energy balance. The
validation of the model under constant and time-dependent
drying conditions showed a good agreement of theoretical
predictions with experimental data in a wide range of stud-
ied parameters (initial solids concentration was set at 20,
30 wt%; air temperature of 67.5, 106.6 C; and air velocity
of 0.45, 1 m=s for constant drying conditions; initial solids
concentration of 20, 30 wt%; air initial temperature of 91.4,
113.4 C; and air ow rate of 30 standard liters per minute
for time-dependent drying conditions; the drying air
humidity was set 0.0001 kg=kg for all cases). The estimated
average differences between the experimental data and
predictions were found to be 1.6 C and 1.1% of weight
for skim milk and 2.0 C and 1.6% of weight for whole milk
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under constant drying conditions. For the time-dependent
drying conditions, these discrepancies were estimated to
be 2.0 C and 1.6% of weight for skim milk and 2.0 C
and 1.1% of weight for whole milk droplets.
It is noted that so far the application of the REA approach
for modeling single droplet drying kinetics have been applied
to the solutions containing skim and whole milk,[17,18,24]
lactose,[25] cream and whey protein concentrate,[26] and
sucrose, maltodextrin DE6, and their mixtures.[28]
A model of particle formation during solution aerosol
thermolysis was proposed by Jayanthi et al.[66] to study
the obtained particle morphology at the evaporation stage
of the process. The authors considered three steps of
spherical particle formation: droplet shrinkage due to
evaporation, transition from shrinkage to constant-
diameter period (also called induction in spray pyrolysis;
see Eslamian et al.[67]), and the constant-diameter period
of thermolysis when all solvent is evaporated. The second
period begins with the onset of precipitation of solid
fraction at the droplet surface and includes subsequent
crystallites appearance inward, from the surface toward
the droplet center. The phenomenon when whole droplet
volume is continuously covered with crystallites during
such the precipitation process was referred by the authors
as volume precipitation. A set of mathematical equations
describing the evolution of uniform droplet temperature
and internal concentration prole in spherical droplet
was derived. Jayanthi et al.[66] adopted the diffusion equa-
tion of concentration prole originally proposed by Char-
lesworth and Marshall,[3] who solved it analytically with
oversimplied assumption of constant droplet diameter.
However, in contrast to Charlesworth and Marshall,[3]
the authors utilized the numerical method developed by
van der Lijn[30] to account for droplet shrinkage during
drying. Further, two necessary conditions for the forma-
tion of fully lled nal particles were formulated. The rst
one is precipitation of the solute in whole droplet volume
(volume precipitation) and the second criterion is concen-
tration of the solute at the droplet center greater than
285
critical value evaluated with the help of percolation theory.
Subsequently, it was suggested that for solutions the
second condition is true if the critical supersaturation con-
centration of the solute is larger than the above-mentioned
critical value. One such solution is a solution of zirconium
hydroxy chloride (ZHC), which was utilized to study the
effects of initial droplet size (the exact studied range is
not indicated; possibly it was up to 50 mm), initial solute
concentration (0.55.7 mol=L), and ambient temperature
(30150 C) on volume precipitation. Also, the inuence
of solute properties was separately investigated. It was
shown that a large difference among the critical supersa-
turation and equilibrium saturation of the solute favored
volume precipitation and, correspondingly, solid particles
formation. Moreover, increase of ambient temperature
reduced the particle density and sometimes led to hollow
particle morphology. In addition, it has been suggested
that low ambient temperatures and initial concentration
of solid content equal to the equilibrium saturation value
promote the formation of dense solid particles. No inu-
ence of droplet initial size on the particle morphology
was observed. The theoretical model predictions were
qualitatively compared with the authors own and available
literature experimental data. These comparisons showed
generally good agreement with model predictions regarding
the obtained particle morphology. Based on comparisons
with experimental data, the authors recommended usage
of ultrasonic atomizers instead of more common two-uid
nozzles because of the extended droplet residence time and
reducing heating rate. However, contrary to what was
expected, the experimental data demonstrated that some-
times low initial concentrations also resulted in solid
particle formation. Jayanthi et al.[66] related this to the
effect of droplet temperature on the critical supersaturation
and equilibrium saturation values, which was neglected in
the model. The authors also noted that further investiga-
tion is needed to determine whether the properties of the
solid crust (thickness, porosity, and mechanical strength)
may also shed light on the experimentally observed forma-
tion of solid particles at low initial solute concentrations.
The model of Jayanthi et al.[66] was recently extended
by Eslamian et al.[67,68] to nanosized droplets and applied
to particle formation by spray pyrolysis and spray-drying
techniques. The basic model equations were the same as
proposed by Jayanthi et al.[66] In contrast, to account
for the nanoscale of the considered droplet, it was postu-
lated that the Knudsen number (ratio of the mean free
path of molecules in the surrounding medium to droplet
radius) would be substantially greater than 0.1 and there-
fore the ow regime should be in a transition range where
the continuum assumption is no longer valid. Correspond-
ingly, a kinetic theory approach was employed to develop
the equation of the droplet evaporation rate. To verify
the model, a zirconium hydroxy chloride solution in
 286 MEZHERICHER ET AL.
nano- and microdroplets of diameter 0.055 mm was sub-
jected to spray pyrolysis at air temperatures between 70
and 400 C in the theoretical and experimental studies.[67]
The successful results of validation allowed the deri-
vation of two semi-empirical correlations for the nal
particle size and wall thickness of obtained ZrO2 parti-
cles as function of reactor pressure, temperature, and
initial solution concentration. Such correlations allow
predicting the expected morphology (either hollow or
fully lled) of the nal particles. At the same time the
authors noted[68] that the formation of highly crystalline
materials, e.g., sodium chloride, follows a different for-
mation mechanism that is not encompassed by the
developed theory. Therefore, further theoretical and
experimental investigations are necessary for comprehen-
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sive understanding of the complex interparticle phenom-
ena occurring during the particle formation.
Discussion
From the literature overview it follows that the most
commonly used modeling approach for the drying of single
droplet with dissolved solids is a combination of species dif-
fusion and assumption of a uniform droplet temperature. A
binary diffusion of liquid (solvent) and dissolved solids (sol-
ute) within the droplet is considered and Ficks law of
diffusion is implemented. The required diffusivity of the
fractions is obtained from experimental measurements.
Further, the widespread assumption of droplet uniform tem-
perature is frequently justied by estimations of a small value
of classical Biot number, but such justication is not always
correct (see discussion of the previous section). Nevertheless,
as shown recently by Patel and Chen,[27] for the majority of
the cases of solution droplets drying except extremal drying
conditions, the assumption of a uniform droplet temperature
provides reasonably accurate predictions of the drying
behavior. These conclusions are also conrmed by the calcu-
lations of Mezhericher et al.[17,18] that were performed for
skim and whole milk droplets using the model that
accounted for the droplet temperature prole. However, in
spite of the acceptable model simplication because of the
uniform droplet temperature, the numerical solution of the
Ficks diffusion equation still requires special treatment[30]
due to the presence of the decreasing droplet radius.
In contrast to the diffusion-type models, an alternative
REA formulation allows avoiding the complicated drying
modeling and resource-consumptive numerical solution.
Moreover, the REA approach is prominent for its high
accuracy. At the same time, due to a sparse database of
materials treated up to now using the REA approach, for
the given liquid solution the investigator most likely will
need costly laboratory facilities to experimentally deter-
mine the necessary functional dependence of the partial
vapor density on the average droplet moisture content.
DRYING KINETICS MODELS SUITABLE FOR BOTH
TYPES OF DROPLETS CONTAINING INSOLUBLE
OR DISSOLVED SOLIDS
Published Models
Parti and Palancz[69] presented a mathematical model
for spray drying in which they analytically treated the dry-
ing kinetics of single droplet=porous particle. The model
equations were developed in general form without making
reference to the droplet type and therefore they can be
applied for droplets with insoluble as well as dissolved
solids. The authors neglected the thermal gradient within
the droplet because of small droplet sizes in the spray
dryer. Moreover, it was assumed that droplet diameter
receded, similar to the shrinkage of a balloon, until the
critical moisture content was attained. After this moment,
the pores were formed inside the particle and its diameter
remained constant. One of the major model deciencies
was the assumption of the saturated particle surface during
the whole drying process, which led to incorrect prediction
of the particle temperature to be constant in the falling dry-
ing rate period. Furthermore, the calculated temperature
gradient between the drying air and particle surface was
abnormally high. For example, simulation of drying of
180-mm particles in the air at 580 C predicted the nal
particle temperature to be equal to only 65 C. It is worth
noting that the model was not validated by any experi-
mental data.
Nesic[11] and Nesic and Vodnik[12] developed a theoreti-
cal drying model of a single droplet containing insoluble or
dissolved solids. The droplet temperature distribution in
both drying stages was neglected. The moisture concen-
tration prole was considered by PDE of Ficks diffusion
and the effect of Stefan ow in the crust pores was disre-
garded. The moisture diffusion coefcient was considered
to be a function of local moisture concentration and the
temperature inuence was ignored. The equation of energy
conservation was developed for quasi-steady-state con-
ditions. A good agreement between the predicted tempera-
ture and mass time change with experimentally obtained
data was observed for colloidal silica and sodium sulphate
droplets. In the case of skim milk droplet drying, the mass
time change showed a ne coincidence with the measure-
ments, but the calculated and experimental droplet
temperatures demonstrated a strong discrepancy in the
second drying stage.
A theoretical drying model of single droplet with
insoluble=dissolved solids developed by Farid[70] was based
on average droplet moisture content. The model took into
account the temperature prole inside the droplet during
the period of initial droplet heating. In the period of
equilibrium evaporation, the droplet temperature distri-
bution was assumed to be uniform and equal to the wet
bulb temperature of the drying air. In the second drying
 MODELS OF SINGLE DROPLET DRYING KINETICS
stage, a common PDE of energy conservation for both
crust and wet core regions of the wet particle was proposed.
The boundary conditions for the particle center and its
surface were given correctly. However, Farid[70] unjusti-
ably assumed that the temperature over the crustwet core
interface was constant and equal to the wet bulb tempera-
ture during drying (similar to Kuts et al.[5]). The thermo-
physical properties of droplet in both drying stages were
assumed to be independent of temperature. Furthermore,
the crust porosity was not taken into account in the heat
balance boundary condition at the crustwet core interface.
In addition to these improper boundary conditions, the
model lacked an essential equation describing the depen-
dence of particle drying rate on the crust resistance to the
vapor mass transfer. Without such a vital equation,
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Farids[70] mathematical model of the second drying stage
led to an unrealistic physical picture, as though the crust
was completely permeable to the diffusion of vapor gener-
ated at crustwet core interface.
Seydel et al.[20,21] utilized a one-dimensional population
balance approach to model the crystallization and distri-
bution of primary particles within the spherical droplet
during the drying process. In this model, the temperature
distribution within the droplet was taken into account.
The authors investigated the inuence of basic drying
parameters like air temperature, initial droplet size, and
initial solids content on the obtained particle diameter
and microscopic solid structure. Free-fall experimental dry-
ing observations of different solutions (inorganic salts) and
suspensions (sodium chloride, ammonium sulphate, and
silica sol) were performed by using droplets with various
initial solid concentrations and changing air temperature
up to 200 C. These experiments demonstrated a micro-
scopic structure of the dried particles and qualitatively
conrmed the results of the corresponding numerical simu-
lations. Despite this, because of the resolution of the
measurement techniques, the authors were unable to carry
out the detailed quantitative model validation.
A computational model of single droplet drying
accounting for the droplet temperature prole in both dry-
ing stages was presented by Dalmaz et al.[71] In their model,
the authors implemented a speculative assumption that the
droplet morphology remained the same during the drying
process; in other words, initial spaces between the primary
solid particles in the droplet remained constant in both dry-
ing stages. In the rst drying stage, this solids frame was
considered to be covered with excess of water. When the
evaporation removed the water excess and uncovered the
solid frame, the second drying stage begun and all the solid
frame was divided into two regions of crust (dry part of the
frame) and internal wet core (part of the frame still lled
with water). Further, in the second drying stage the drying
was assumed to occur under the crust by means of vapor
diffusion from the wet core though the pores lled with
287
air. Correspondingly, one energy balance PDE and one
mass balance equation were derived for the rst drying
stage, and two energy balance PDEs for crust and wet core
and one Ficks diffusion law PDE for the crust pores were
developed for the second drying stage. Moreover, vapor
concentration over the droplet and particle wet core region
was estimated using the saturation conditions. To validate
the proposed model, simulations of silica and skim milk
droplets drying behavior were performed and the obtained
results were compared to Nesic and Vodniks[12] experi-
mental data. The validation demonstrated a satisfactory
agreement of the predicted silica droplet average tempera-
ture and mass evolutions with the experimental for air
temperature of 101 C. However, it must be noted that
the adopted assumption about the constant droplet
morphology in both drying stages forced the authors to
set an extreme value of the particle porosity of 0.588 in
order to t the experiment. Consequently, taking into
account that the utilized silica primary particles were
monosized and equal to 16 nm in diameter, it is unclear
how they can compose the nal solid spherical particle with
such a great porosity. Moreover, a maximal difference of
13 C between the silica particle surface and center was pre-
dicted, whereas Mezhericher et al.[17] estimated this value
to be up to 3.5 C. Dalmaz et al.s[71] simulations of skim
milk droplet drying at 50 C demonstrated worse coinci-
dence with experimental temperature than silica, especially
in the rst drying stage. Admittedly, this discrepancy was
due to unsuitability of assumption of saturated vapor
concentration over the droplet in the rst stage and particle
wet core in the second drying stage, skim milk is not a
suspension. Furthermore, the authors once again presumed
an extreme particle porosity of 0.651 in order to t the
measurements. Finally, 10 C of temperature difference
between the skim milk particle surface and its center was
calculated, which subsequently diverges from negligible
temperature differences observed by Mezhericher et al.[17]
and Patel and Chen[27] for skim milk droplets dried at
temperatures up to 106.6 C.
Recently, Handscomb et al.[22,23,72,73] developed a theor-
etical drying model of a single droplet containing a com-
plex multicomponent mixture. The mixture consisted of a
continuous phase of an ideal binary solution and a discrete
phase of insoluble suspended solids. Three components
were considered: solvent, solute, and solids. As the result
of drying, the solute from the continuous phase could not
deposit to increase the solids quantity. Similarly to Seydel
et al.,[21] the behavior of the discrete solid phase was
described by a population balance of spherical particles
of different diameter and location within the droplet. The
continuous phase was modeled by a volume-averaged
differential mass balance of the solute assuming Fickian
diffusion for the transport term. The effect of Stefan ow
was disregarded in the mass ux of moisture from the
 288 MEZHERICHER ET AL.
drying droplet. A uniform droplet temperature was
presumed in both drying stages. The formation of the crust
was deemed to occur once the solids volume fraction at the
droplet surface rose above a predened critical value. In
contrast to most of the published models, the authors did
not presume an immediate droplet shrinkage cessation
after the onset of crust formation. Correspondingly, the
model provided for a shell-thickening regime with droplet
shrinkage between the beginning of crust formation and
establishment of a rigid crust. Such rigid crust has a critical
thickness when the shrinkage ceases and represents the bal-
ance of collapsing capillary forces and crust structural
strength. Furthermore, the authors subdivided the rigid
crust into two types, dry shell and wet shell, which were
determined by the mechanism of moisture transport.
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Consequently, a wet particle with a dry shell has no
continuous phase remaining in the completely dry crust
region and evaporation occurs from the receding interface
between the crust and wet core regions. Unlike this, the wet
shell approach implies the crust is wetted by a continuous
phase, evaporation from the crust outer surface, and a sin-
gle vapor bubble located in the droplet center. Handscomb
et al.[23,72] reported the successful validation of the developed
model in the rst drying stage. The authors compared the
calculated evolution of droplet temperature and mass until
the moment of crust formation with published experimental
results. They used available drying data of pure water[74] and
colloidal silica and sodium sulphate[12] single droplets. In
their subsequent work, Handscomb et al.[22,73] studied the
drying behavior of two single droplets in both drying stages.
In this research, a detergent slurry (crutcher mix) was
assumed to form a dry shell crust and a colloidal silica drop-
let was supposed to form a wet shell region. The dry shell
assumption was supported by Grifth et al.s[75] experi-
mental study of detergent droplet drying. Additionally,
though it was not mentioned by the authors, the presump-
tion of wet shell formation in the silica droplet with 16-nm
primary particles can be conrmed by experimental observa-
tions of Walton and Mumford,[50,58] who found that for
agglomerate-forming materials like silica or carbon, the nal
granules tended to be solid if the size of primary particles
was >>1 mm and hollow if the primary particles were smaller
than 1 mm. The results of detergent slurry drying simulation
showed a good agreement with experimental evolution of
moisture mass fraction and moisture proles measured by
Grifth et al.[75] using magnetic resonance imaging techni-
ques. Despite this, the experimental proles of moisture con-
tent indicated that an extension to the proposed dry shell
approach may be required because a certain fraction of the
crust pores possibly remained lled by the continuous phase
during drying. Another arguable prediction of the model is
that the simulated evolution of the solids volume fraction
demonstrated a negative solids gradient immediately under
the crust region (as if there was a sink of solids). Moreover,
the calculated evolution of the detergent droplet temperature
was not presented and was not validated by the authors.
The results of simulations of colloidal silica droplet drying
using the wet shell approach demonstrated a good t to
the measured evolution of the droplet mass[12] at the studied
drying air temperatures of 101 and 178 C. Unlike this, the
rate of the droplet temperature rise in the second drying
stage was underpredicted in air of 101 C and it was
explained by the model assumption of a uniform droplet
temperature. Furthermore, the model overpredicted the rate
of the droplet temperature growing in air of 178 C and
doubtfully suggested the initiation of boiling within the
droplet when its temperature reached 100 C. The last pre-
sumption should be justied by the values of vapor pressure
over the droplet surface and water concentration in the
droplet interior.
The model developed by Handscomb et al.[22,23,72,73] has
also been utilized by Handscomb and Kraft[76] to test its
capability of simulating different particle morphologies.
The authors proposed several criteria for choosing the
appropriate structural submodel (shell thickening, dry
shell, wet shell, slow boiling) to be used for the specic
droplet drying simulation. The developed criteria were
incorporated into a decision algorithm based on the com-
parative analysis of the droplet inner pressure and the crust
strength during drying. To demonstrate the capability of
the algorithm, simulations of a colloidal silica droplet dry-
ing in air at 101 and 178 C were performed. The presented
results of silica drying at 178 C indicated the formation of
a full nal silica particle without a central void. However,
using the same drying model and the same drying con-
ditions as reported by Handscomb et al.,[23,73] the authors
predicted the formation of a hollow silica particle. These
confusing contradictions in the morphology predicted for
the same drying case by the same drying model were not
explained. Further varying the size of suspended silica par-
ticles in the range of 02000 nm, the authors investigated its
inuence on the nal particle morphology at air tempera-
ture of 178 C. It was established that the solid nal parti-
cles were produced if initial droplets contained primary
particles with size up to 50 nm; droplets containing solids
with size between 50 and 1000 nm turned into the hollow
nal particles and droplets with silica particles larger than
1 mm again were dried into the solid particles without
central void. These theoretical predictions, except for the
suspended particles sizes smaller than 50 nm, were also con-
rmed by experimental observations reported by Walton
and Mumford.[50,58] Combining the results from multiple
simulations of colloidal silica droplet drying in air at
178 C, Handscomb and Kraft[76] constructed a map illus-
trating the connection between the suspended particle size
and the predicted dried particle morphology.
During recent years, Mezhericher et al.[1719,42,77] theore-
tically investigated the process of single droplet drying with
 MODELS OF SINGLE DROPLET DRYING KINETICS
the focus on wet particle cracking=breakage in the second
drying stage.
In the study of Mezhericher et al.,[17] a two-stage drying
model assuming temperature prole within the droplet in
the both drying stages was compared with the approach
accounting for the internal temperature distribution only
in the second drying stage. The developed formulation
assumed spherical solid nal particle formation, ideal
mixing between liquid and solid fractions, and absence of
internal circulation in the droplet. The process of droplet
drying in the rst drying stage is considered to be similar
to the evaporation of a pure liquid droplet. Subsequently,
when the droplet average moisture content decreases to a
predened critical value, the formation of porous crust
commences at the outer droplet surface and the droplet
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turns into a wet particle with constant outer diameter
and wet core, which shrinks due to vapor diffusion via
the crust pores (this viewpoint is also supported by the
experimental observations of Yarin et al.[36]). Correspond-
ingly, in the second drying stage the temperature prole in
the crust and wet core regions was modeled by an energy
conservation PDE and Abuaf and Staubs[9] equation for
the mass transfer rate of diffusing vapor through the crust
pores was adopted. To enable the drying kinetics predic-
tion for the droplets containing dissolved solids, the density
of vapor over the droplet surface was calculated using the
REA approach.[24] To validate the developed model, its
theoretical predictions were compared to experimental data
of silica[11] and skim milk droplet drying.[78] The thermo-
physical properties of silica were assumed to be tempera-
ture independent, whereas the properties of skim milk
components were evaluated according to Chen and Peng[79]
as temperature functions. The results of numerical simula-
tions showed a good agreement between the predicted and
experimental temperature and mass histories of silica drop-
let drying. Furthermore, the calculations predicted a grow-
ing temperature difference between the silica particle outer
surface and its center in the second drying stage. Thus, at
the end of the silica drying this difference was found to
be up to 3.5 C when drying air temperature was set to
101 C and up to 22 C at air temperature of 178 C. For
skim milk drying simulations at air temperature of
67.5 C, the maximum discrepancy between predicted and
experimental temperatures did not exceed 5%, whereas
the differences between corresponding mass values were
lower than 4%. The temperature difference between the
particle outer surface and its center was found to be negli-
gible in this case. In general, it has been established that the
droplet temperature prole can be disregarded in the rst
drying stage, whereas in the second drying stage the
temperature difference can attain considerable values in
the particle crust (depending on drying conditions and
crust thermophysical properties) and while it remains small
in the wet core region.
289
In subsequent research, Mezhericher et al.[18] aimed to
investigate the inuence of previously found temperature
gradient in the crust of silica particle[17] on the potential
particle cracking=breakage during intensive drying. For
this purpose, the previously developed model was enhanced
by accounting for forced vapor ow in the crust pores
because of pressure difference between the wet core and
outer surface of the particle. The performed drying simula-
tions of silica and whole milk droplets demonstrated a
reasonable agreement with literature experimental data.
For the considered drying conditions, the model predicted
substantial temperature gradients in the silica and
negligible in the whole milk. Based on these ndings, the
presence of thermal stresses in the silica crust was postu-
lated. Treating the crust region as a pseudo-porous spheri-
cal container, a distribution of thermal stresses in the crust
of the silica particle was mathematically described and
numerically calculated for different drying conditions (air
temperature was set to 150750 C, air velocity was chan-
ged in the range 0.51.5 m=s) and various initial silica drop-
let diameters (between 10 and 2000 mm). It was found that
tangential thermal stress in the wet particle crust was
predominant over the radial component (approximately
4.5 times more for silica granules in broad range of drying
conditions). To predict the cracking=breakage of the silica
particle crust, a failure criterion was proposed. This par-
ticle breakage criterion is based on two well-known failure
criteria for brittle materials; i.e., maximum normal stress
criterion and Mohrs theory. According to the suggested
formulation, the silica particle breakage can be expected
to occur if one of the largest radial or tangential tensile
thermal stresses will be greater than particle crust tensile
strength. Further, it was assumed that the tensile strength
of particle crust was equal to the upper bound of agglom-
erate strength due to van der Waals forces, which in turn
are strongly dependent on the size of primary particles
composing crust.[80] Using these values of estimated
particle crust strength as a function of primary particle size
and the values of calculated thermal stresses for various
silica granule diameters as a function of drying air tempera-
ture, a map was constructed that allows predicting whether
the breakage of silica particles will occur under the given
drying conditions.
The continuing study of Mezhericher et al.[19] was
devoted to investigation of fully unsteady character of heat
and mass transfer in the second drying stage. Distinct from
the previous works,[1719] the developed elaborate model
considered a completely unsteady character of heat and
mass transfer in the second drying stage and enabled calcu-
lation of the pressure and vapor fraction proles within the
capillary crust pores by the set of corresponding PDE. The
model equations were numerically solved based on
a predictor-corrector method and simulations of single
silica droplet drying have been performed. To verify the
 290 MEZHERICHER ET AL.
developed model under different drying conditions,
comparisons between the drying histories of the silica drop-
let with the data calculated utilizing the previous model[18]
were performed and they proved insignicant discrepancies
between the two models for both droplet temperature and
droplet mass evolutions. In the subsequent numerical stu-
dies, the drying air temperature, drying air velocity, initial
droplet diameter, and porosity of the particle crust were var-
ied in wide ranges (air temperature was set to 150750 C, air
velocity varied between 0.25 and 3.5 m=s, droplet initial
diameter was 0.252 mm, and particle crust porosity was
altered in the range 0.10.4). One of the signicant ndings
was the continuous rising of the pressure over the crustwet
core interface (under the particle crust). This model
prediction was explained by imbalance of two concurrent
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processes: vapor mass ow inside the pores by diffusion
and forced mechanisms toward the particle outer surface
and, on the other hand, diffusion of the dry air from the sur-
rounding medium inward the particle and simultaneous
forced ow of dry air in the opposite direction. Analyzing
the results of calculations, it was also concluded that in the
studied cases the diffusion mechanism of vapor ow in capil-
lary pores played a more substantial role than the pressure-
driven vapor ow. Moreover, the developed model predicted
that liquid boiling inside the silica particle wet core did not
occur even at elevated drying temperatures (up to 750 C)
because the wet core temperature remained lower than the
liquid saturation temperature corresponding to the wet core
pressure. It is worth noting that at the present time one of
the model drawbacks is its extended requirements regarding
the computation time. Such a disadvantage will be reduced
with further progress in the computer technology.
Using the ability of the advanced droplet drying kinetics
model by Mezhericher et al.[19] to predict the temperature
and pressure proles within the droplet, this model was
later extended by the authors to account for both thermal
and mechanical stresses emerging in the second drying
stage. The model, recently reported by Mezhericher
et al.,[42] incorporated the effect of heat transfer due to
thermal radiation as well. Such a modication was made
in order to generalize the theoretical description, because
Mezhericher et al.[77] demonstrated that for small initial
droplet diameters up to 0.25 mm and ambient temperatures
<750 C as well as for initial droplet diameters <2.5 mm
and ambient temperatures up to 200 C, the effect of ther-
mal radiation can be neglected; but for droplets with initial
diameter greater than 1 mm and temperatures of the drying
agent higher than 400 C, thermal radiation plays a
substantial part in the drying process and must be taken
into consideration. Similar to the study of Mezhericher
et al.,[19] it has been suggested that van der Waals forces
are the dominating binding mechanism between the pri-
mary particles in the crust of a slurry droplet during the
second drying stage. However, in contrast to the previous
study, the particle breakage criterion became more sophis-
ticated because it took into account the total drying stress
including components of both thermal and mechanical
stresses. According to the improved breakage criterion,
the nal particle of slurry droplet is predicted to be
damaged if one of the total stress components in the crust
is greater than the crust agglomerate strength determined
by the van der Waals forces binding mechanism. The con-
ducted numerical simulations of silica drying demonstrated
that mechanical stresses played a substantial role at the
beginning of the second drying stage, but at the end of
drying the thermal stresses appeared to be much more con-
siderable. It was also found that the total tangential stress
in the crust of wet silica particle prevailed over the radial
component (approximately ve times greater during
drying). Similar to Mezhericher et al.,[19] by comparing the
calculated stresses to the improved breakage criterion it
has been concluded that the total stresses can result in
particle cracking=breakage and depend on granule diameter,
drying agent temperature, and diameter of primary particles.
An improved, elaborated map of silica particle breakage
accounting for the calculated total stresses was constructed.
With the help of the map, the authors suggested that in
order to prevent the granule breakage at given drying con-
ditions, the slurry droplets must contain primary particles
as small as possible.
Discussion
The drying kinetics models suitable for both types of
droplets containing insoluble or dissolved solids are promi-
nent for elaborate equations, exibility, and universality of
application. A literature overview shows their other out-
standing characteristics like the ability to predict tempera-
ture, species, and pressure distributions; calculation of
emerging thermal and mechanical stresses leading to the
product damage; and evaluation of the obtained particle
structure and morphology. But these favorable features
are disbursed by the complexity of the theoretical formu-
lation and corresponding difculty of the numerical
solution. Furthermore, at the present time the numerical
simulation of single droplet drying using the discussed
model type can involve many computer hours and even
several days. Fortunately, with the current rate of the com-
puter advancements this running time will be substantially
reduced within the next few years.
Based on the literature survey, the prospective modeling
effort for the drying kinetics of single droplet containing
insoluble or dissolved solids is to enable the prediction of
the structure and morphology of the obtained nal
particles from the initially multicomponent material. In
addition, it is important to consider the internal stresses
that will facilitate the comprehensive understanding of
the reasons leading to the product degradation during the
real drying processes.
 MODELS OF SINGLE DROPLET DRYING KINETICS
SUMMARY AND CONCLUSIONS
During recent years a growing interest in theoretical and
experimental investigations of single droplet drying has
been encouraged by the requirement of comprehensive
understanding of the drying phenomena in such extensively
used technological processes like spray drying, uidized
bed drying, pneumatic drying, etc.
In the present article, different approaches for modeling
of droplet drying kinetics have been overviewed. The mod-
els were identied to be suitable for droplets with insoluble
solids, for droplets with dissolved solids, and for droplets
containing both types of solid content.
Key transport phenomena during droplet drying like
convective heat and mass transfer to and from the drop-
let, conductive heat transfer, and moisture diffusion
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accompanied by the droplet shrinkage and porous crust
formation within the droplet were indicated in this review.
Further fundamental theoretical investigations validated
by experimental measurements are still essential for the
comprehensive understanding of the single droplet drying
phenomenon, especially for realistic predictions of the
obtained particle structure and morphology as well as
development of practical recommendations allowing to
avoid the cracking and rupture of wet particles leading to
degradation of the nal product.
ACKNOWLEDGMENT
The authors acknowledge the nancial support of the
present work from GIF (German-Israeli Foundation for
Scientic Research and Development) under Grant No.
952-19.10=2007.
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