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Computer Modeling of Sugar Crystallization During Drying of Thin Sugar Films

Computer Modeling of Sugar Crystallization During Drying of Thin Sugar Films

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*
Corresponding author. Fax:
#
1 608 263 1965; e-mail:hartel
@
calshp.cals.wisc.edu.Journal of Crystal Growth 198/199 (1999) 1294
— 
1298
Computer modeling of sugar crystallization during dryingof thin sugar films
E. Ben-Yoseph, R.W. Hartel
*
 Department of Food Science, Uni
v
ersity of Wisconsin, 1605 Linden Dri
v
en, Madison, WI 53706, USA
Abstract
A computer model was developed to predict drying and crystallization during processing of thin sugar films underthe conditions of importance for sugar-coated cereals. The three-dimensional model analyzed simultaneous heat andmoisture transfer, accounting for shrinkage, with temperature and moisture-dependent transport properties. Crystalgrowth was evaluated from crystallization kinetics based on supersaturation and temperature. The influence of growthon the solution concentration and drying were taken into account. Concentration profiles around the growing crystalsduring drying of the thin films were evaluated. The model predicts a concentration reduction around the growingcrystals, and film temperatures that are higher than the drying temperature (as a result of the release of fusion heat).A phenomenon of case hardening was observed for dried films with a high density of seeds on surface.
1999 ElsevierScience B.V. All rights reserved.
 Keywords:
Crystallization; Drying; Sucrose; Sugars; Modeling; Films
1. Introduction
Controlling crystallization of sugars in thin filmsis critical to development of the proper appearanceof sugar-coated cereal products. In this process,a thin sugar film is applied to the surface of a cerealpiece,and then allowed to dry. By proper control of the crystallization and drying processes, the appro-priate appearance, either frosted or glazed, canbe developed. However, our understanding of theparametersthat influencethese processes,for devel-oping a specific appearance, is severely lacking.Cereal companies have problems getting consistentresults with this process. Usually, the film is frostyat the end of the process, which is the desiredappearance. However, sometimes the appearance isglossy, which is undesired.The objective of this work was to develop a com-puter model for predicting crystallization kineticsduring drying of thin sugar films under the condi-tions of importance for sugar-coated cereals. Thisincludes developing a three-dimensional modelthat evaluates changes in all dimensions within thefilm, evaluating the concentration profile around
0022-0248/99/$
— 
see front matter
1999 Elsevier Science B.V. All rights reserved.PII: S0 0 2 2 -0 24 8 (9 8 ) 01 0 1 4- 8
 
the growing crystals, and accounting for crystalsgrowing together. The simulation program deter-mined the crystal size, shape and distribution in thefilm. Using this information,the final appearanceof the film, either frosty or glassy, will be predicted inthe next phase of the study.
2. Theory
,
modeling and experimental procedure
2.1. Computer simulation of drying process
Okazaki et al. [1] presented the mass transferequationin a one-dimensional,twocomponentsys-tem with shrinkage, assuming all moisture move-ment was by diffusion. This equation was expandedto three dimensions, since crystal growth is athree-dimensional phenomenon, to get
jj
Ct
"
jj
x
D
V
X
R
jj
Cx
#
xS
V
jj
S
V
t

jj
Cx
!
2
D
V
C
#
C
1
S
V
X
R
jj
Cx
#
jj
y
D
W
½
R
jj
Cy
#
yS
W
jj
S
W
t

jj
Cy
!
2
D
W
C
#
C
1
S
W
½
R
jj
Cy
#
jj
z
D
X
Z
R
jj
Cz
#
zS
X
jj
S
X
t

jj
Cz
!
2
D
X
C
#
C
1
S
X
Z
R
jj
Cz
, (1)where
C
is the dimensionless moisture in film and
t
is time.
C
,
C
and
¼
are defined as follows:
C
"¼

¼


,
C
"¼

¼


,
¼
"
!
, (2)where,
¼
is the mass fraction of water,
¼

isthe equilibrium water mass fraction,
¼

is theinitial water mass fraction,
is the density of purewater,
is the density of pure sucrose.
x
,
y
, and
z
are dimensionless depth into the box in the
x
,
y
,and
z
directions, respectively, defined as
x
"
XX
,
y
"½½
,
z
"
ZZ
(3)where
X
,
½
, and
Z
are the depth into the box in the
x
,
y
, and
z
directions, respectively, and
X
,
½
, and
Z
are the thickness of the box in the
x
,
y
, and
z
directions, respectively, as a function of time.
D
V
,
D
W
and
D
X
are the mutual diffusion coefficients inwater-sucrose system in the
x
,
y
, and
z
directions,respectively.
S
V
,
S
W
, and
S
X
, arethe shrinkagemagni-tude of the box in the
x
,
y
, and
z
directions.The initial conditions describe the temperatureand concentration of the solution at the beginningof the process:at
t
"
0 for all
i
,
j
, or
k
:
C
G
H
I
"
1, (4)at
t
"
0:
S
"
1,
¹"¹
, (5)where
i
,
j
, and
k
are subscripts which refer to nodesin the grid point system in the
x
,
y
, and
z
directions.The boundary conditions supply information onexternal conditions surrounding the solution,which affect the behavior of the surface solutiontemperature and heat and mass transfer rates dur-ing drying. The boundary conditions used werefor
z
"
0 and
t
'
0:
jj
Cz
"
0 (6)for
z
"
1 and
t
'
0:
!¼
(
C
#
C
)
D
X
SZ
j
C
j
z
"
k
E
(
P
!
P
) (7)
!
d
S
d
t
"
k
Z
(
P
!
P
) (8)[
m
c
#
c
Z
X
½
(
!
)
#
c
Z
X
½
(
!
)
#
c
Z
X
½
S
]d
¹
d
t
"
h
X
½
(
¹
)
#
r
Z
X
½
d
S
d
t
, (9)where,
is the solution density,
k
is the masstransfer coefficient at the solution surface,
P
isthe partial pressure of water vapor at film surface,
 E. Ben-Yoseph, R.W. Hartel 
/
Journal of Crystal Growth 198
/
199 (1999) 1294–1298
1295
 
P
is the partial pressure of water vapor in hot air,
m
is the mass of the flake,
c
is the heat capacity of the flake,
c
is the heat capacity of sucrose,
c
is theheat capacity of water,
is the initial density of solution,
is the water density at the initialsolution temperature,
r
is the latent heat of vapor-ization of water,
h
is the heat transfer coefficient atfilm surface,
¹
is the solution temperature and
¹
isthe drying air temperature.Calculating the temperature only as a functionof time, and not as function of location, we assumethat the temperature distribution is negligiblysmall because of the film being very thin and thereis no convection flow in the film at this high visco-sity of the solution. Furthermore, the thermaldiffusivity of sucrose/water system in high concen-tration of sucrose, as given by Bhowmik andHayakawa [2] and by Hayakawa and Bakal [3], is3 fold higher than the mass diffusivity of thesystem.The resulting system of nonlinear partial differ-ential equations in time and three dimensions weresolved numerically by applying the finite differencemethod. In the classical finite difference applica-tion, the distance between the nodes is constant.However, since shrinkage is not negligible duringdrying (the film shrinks when dried at a rate de-pending upon the solution concentration and thedegree of drying) the physical dimension of the filmis changing during drying. Therefore, the variablegrid central finite difference method was applied[4,5].The physical parameters used during calcula-tion were assumed to be functions of local con-centration and/or temperature. These parameterswere defined explicitly from several literaturesources.
2.2. Predicting the state of solution,
and crystalgrowth rate
,
size
,
shape and distribution
The information about temperature and concen-tration at any location in the film during the dryingprocess located each point in the film in the phasediagram; either it is an undersaturated, metastable,labile or glassy solution.A region in the film was considered glassy if itstemperature reached below the glass transitiontemperature,
¹
, during the drying process. Roosand Karel [6] gave a method to calculate
¹
forsucrose by applying the Gordon and Taylor equa-tion:
¹
"
w
¹
#
kw
¹
w
#
kw
, (10)where
w
and
w
are weight fractions of componentcompounds,
¹
and
¹
are the absolute glasstransition temperatures (K) of the componentcompounds, and
k
is a constant. In our case,
¹
"
138 K (
¹
of water),
¹
"
335 K (
¹
of puresucrose), and
k
for sucrose
— 
water equal to 4.7.For supersaturated, non-glassy solution, themodel calculated the supersaturation level asa function of the local concentration and the satu-rationconcentration(which is a function of temper-ature). The growth rate of sugar crystals as afunction of the supersaturation level and temper-ature was calculated from a sucrose growth modelbased on data given by Hartel et al. [7]. Regressionfrom this data (
R
"
0.9697), gave the followingequation, valid for temperature range of 44
— 
54
°
Cand supersaturation ratio above 1.0576:
G
"
7.0538
S
!
7.46, (11)where,
G
is the growth rate for a single crystal(
m/min) and
S
is the supersaturation ratio (con-centrations of grams sucrose per grams of water).
2.3.
v
aluation of the crystal growth in
 fl
uenceon the
lm
All the following phenomena were taken intoaccount in the simulation program:(1) Reduction in concentration: when a crystalgrew, sucrose was removed from the solution andthe concentration around the crystal decreased.The change in concentration was calculated frommass balance of sucrose and water.(2) Generation of fusion heat: when a crystalgrew, it generated heat that raised the film temper-ature. An additional term was added to the heattransfer equation, relative to the amount of massthat was built on the crystal [8].(3) Decrease in diffusivity: the volume of a crys-tal acted as a barrier for diffusion of sucrose andwater. To model this influence, a mass transfer of 
1296
E. Ben-Yoseph, R.W. Hartel 
/
Journal of Crystal Growth 198
/
199 (1999) 1294–1298

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