Innovative Food Science and Emerging Technologies 7 (2006) 225 232 www.elsevier.

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Computer simulation of sugar crystallization in confectionery products

Eyal Ben-Yoseph a,, Richard W. Hartel b,1
b

15 Hurshat Tal Street, Yokneam, Israel Food Science Department, University of Wisconsin, 1605 Linden Drive, Madison, WI, USA Received 11 May 2005; accepted 2 December 2005

Abstract A computer simulation was developed to model drying, moisture sorption and crystallization, during processing and storage of confectionery products. The three-dimensional model analyzed simultaneously heat and moisture transfer, accounting for shrinkage, with temperature and moisture-dependent transport properties. Kinetics of crystal growth at different solution conditions were determined experimentally. Predicted crystal growth rates were evaluated from crystallization kinetics based on supersaturation, temperature, and state of the solution. The influence of growth on the solution concentration and drying rate were taken into account. The model predicted quality and storage stability based on correlations with the calculated sugar concentration, crystallinity and phase state. Simulation results were in agreement with theory and experimental results. 2006 Elsevier Ltd. All rights reserved.
Keywords: Sugar; Crystallization; Confectionery; Drying; Modeling Industrial relevance: The goal of this work was to develop a model for quality and storage stability determination of confectionary products using crystallization of sugar shell in hard panning process as example. The model developed can successfully predict the concentration profile and growth of sugar crystals in a thin film and its industrial relevance is evident by the industrial financial support.

1. Introduction Controlling crystallization of sugars in confectionery products is critical to development of their proper appearance, texture and storage stability (Hartel, 2001). Sugar crystals in the product may be desirable (e.g. sugar shell, fondant, toffee and fudge), or undesirable (e.g. hard candy, jelly and caramel). However, our understanding of the parameters that influence those attributes is severely lacking, since heat transfer, mass transfer, and phase transition phenomena, which determine crystallinity, are complex and interrelated. A computer simulation can model these phenomena, and predict crystallization during the production process and storage of confectionery products. The use of computer simulation can result in
Corresponding author. Tel.: +972 4 993 7052; fax: +972 4 959 7631; mobile: +972 5 378 2036. E-mail addresses: em@carmel-consulting.com (E. Ben-Yoseph), rwhartel@wisc.edu (R.W. Hartel). 1 Tel.: +1 608 263 1965; fax: +1 608 2626872. 1466-8564/$ - see front matter 2006 Elsevier Ltd. All rights reserved. doi:10.1016/j.ifset.2005.12.003

faster and cheaper process development, help optimize existing processes, and improve our understanding of the product properties. The objective of this work was to develop a model that determines quality and storage stability of confectionery products. We chose to model the simplest confectionery system, i.e., sucrose solution, which is applied as a thin film on a solid surface as might be found in a panned confection. The quality attribute modeled was the appearance of the coating, which was directly related to the surface area coverage of crystallinity of the coating. Storage stability was predicted based on the water activity and glass transition temperature. The model in its current configuration can be used to model crystallization of sugar shell in Hard Panning process. For more complex systems, the model needs to be modified. For example, to model a system of sucrose, corn syrup and water (e.g. Hard Candy) the governing equations need to be changed; namely for diffusivity of sucrose and water, glass transition temperature equation, water activity equation and sucrose crystallization kinetics in the presence of corn syrup.

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2. Theory/modeling The modeling phase consisted of the following eight major steps: 1. The temperature of the film as function of time was calculated from the heat transfer equation. 2. The sugar concentration as function of time and location was calculated from the unsteady state mass transfer equation. 3. Crystal growth rate at each spatial point in the film was predicted based on local supersaturation, film temperature, and growth kinetics. Rate of crystal growth as function of supersaturation and temperature was used from previous data (Howell & Hartel, 2001) 4. Crystal size was calculated based on the crystal growth rate at each point in space and time. 5. The influence of crystal growth on the film concentration and temperature was evaluated. 6. Glass transition concentration was calculated from the film temperature, and local amorphous areas within the film were defined. At this point we were able to define three different regions in the film: (a) crystalline region its amount, location, and crystals number and size; (b) solution region amount, location, and the concentration profile; and (c) amorphous region its amount, location, concentration, and the glass transition temperature. This information was used in the last 2 steps of model development: 7. Crystal area coverage was predicted from the crystal size and distribution in the film. 8. Storage stability was predicted based on glass transition temperature and water activity, which were calculated from
Initial conditions Process conditions

the sugar concentration of the solution phase and the amorphous phase. The working steps are illustrated in Fig. 1. 2.1. Heat and mass transfer The system of nonlinear partial differential equations for heat transfer in time and for mass transfer in time and three dimensions was solved numerically. The sucrose solution was subdivided into many small rectangular elements in order to apply the finite difference method. A detailed description of the methodology used to predict the temperature and concentration in the film are found in Ben-Yoseph, Hartel and Howling (2000). Many of the physical parameters within the film are functions of local temperature and/or concentration. These parameters were defined explicitly and are listed in Table 1. 2.2. Predicting the state of solution, and crystal growth rate, size, shape and distribution The information about temperature and concentration at any location in the solution during the drying process located each point in the solution in the phase diagram; either it was an undersaturated, metastable, labile or glassy solution. A region was considered glassy if the temperature at that point was below the glass transition temperature, Tg. Roos and Karel, 1991 suggested a method to calculate Tg for sucrosewater by applying the Gordon and Taylor equation: Tg w1 Tg1 kw2 Tg2 w1 kw2 1

where w1 and w2 are weight fractions of component compounds, Tg1 and Tg2 are the absolute glass transition
Correlation of physical properties to solution conditions

(1)
Numerical solution of Heat Transfer Equation (1)
T(t)

Numerical solution of Mass Transfer Equation (2)

C (t,x,y,z) S(t)

(5)
Growth influence on solution

Experiments of crystal growth (with Howell)

Crystallization kinetics

(3)
Crystals size, shape and location, glass transition concentration

(4,6)

(7)
Crystal coverage

(8)
a w , Tg

Fig. 1. Schematic illustration of the working steps, as described in this section. The numbers in parenthesis correspond to the steps described in Section 3.

E. Ben-Yoseph, R.W. Hartel / Innovative Food Science and Emerging Technologies 7 (2006) 225232 Table 1 Physical properties of water, sucrose, sucrose solution and air, as a function of temperature and/or concentration Properties (source) Density of sucrose solution (Honig, 1953) Density of pure water (Geankoplis, 1983) Density of pure sucrose (Reiser, Birch, & Mathlouthi, 1995) Solubility of sucrose in water (Pancoast & Junk, 1980) Vapor pressure of pure water (Perry & Chilton, 1973) Relative vapor pressure of water above sucrose solution (Norrish, 1966) Heat capacity of sucrose (Honig, 1953) Heat capacity of water (Geankoplis, 1983) Heat of fusion for sucrose (Pancoast & Junk, 1980) Heat of vaporization of water (Felder & Rousseau, 1986) Air density (Geankoplis, 1983) Air viscosity (Geankoplis, 1983) Air thermal conductivity (Geankoplis, 1983) Diffusivity of water vapor in air (McCabe, Smith, & Harriot, 1985) Units g/mL g/m3 g/m3 % w/w sucrose mm Hg mm Hg cal/g/C cal/g/C cal/g cal/g g/mL Ranges and parameters units Correlation 333373 K 60100% TS 50100 C C 090 C 323373 K 323373K 0100% TS 0100 C 50100 C 65.693.3 C 5080% TS 10100 C 0100 C

227

= [1.2351 7.52 * T * 10 4 + (2.74 + 0.002625 * T ) * TS * 10 3 + (2.35 0.00175 * T ) * TS2 * 10 5] * 10 6 w = [1.0045 1.9582 * 10 4 * T 2.6589 * 10 6 * T 2] * 10 6 s = (1.5887 4.4285 * 10 5 * T ) * 10 6 S = 64.397 + 0.07251 * T + 0.0020569 * T 2 9.035 * 10 6 * T 3 (12.73475940.0089/(230+T)) P0 w = 10 Ps,w = [0.671 0.3355 * log10(TS)] * P0 w cs = 0.2619 + 1.2858 * 10 3 * T cw = 1.0017 1.5754 * 10 4 * T + 2.1607 * 10 6 * T 2 Hf = 0.0551 * TS + 0.1988 * T 4.0902 rw = 598.34 0.58456 * T g = 1.2910 * 10 3 4.4026 * 10 6 * T + 9.4193 * 10 9 * T 2 g = 1.7355 * 10 4 + 4.4309 * 107 * T = 5.7889 * 10 5 + 1.7840 * 10 7 * T Dv = 3.22 * 105 * T 1.81

g/cm/s 40120 C cal/s/cm/K 0100 C ft2/h p = 1 atm T = [K]

temperatures (K) of the component compounds, and k is constant. In our case, Tg1 = 138 K (Tg of water), Tg2 = 335 K (Tg of pure sucrose), and k for sucrosewater equal to 4.7 (Roos & Karel, 1991). Growth kinetics of sucrose crystals were studied in a method described by Howell, Ben-Yoseph, Rao and Hartel (2002), and the results were correlated to the solution conditions using the following equation (Wey, 1981): G 2DAB C Ci rs d 2

with concentration. The growth rate is zero when the supersaturation equals zero or when the diffusivity equals zero. Plotting the growth rate as function of concentration gives a convex curve with a maximum growth rate at a specific solution concentration. During growth, when the volume of a seed reached the element volume, growth continued in the adjacent elements (as long as there were no crystals in these elements). Growth continued from the center of the adjacent element (Fig. 2) with growth rate proportional to the surface concentration in this volume element. One or more seeds can be placed at any point in the matrix. 2.3. Evaluation of the influence of crystal growth on the temperature and concentration Sugar crystals growing within the solution exert an influence on the surrounding environment. The following phenomena were taken into account in the simulation program: 1) Reduction in concentration: When a crystal grew, sucrose molecules were removed from the solution and the concentration around the crystal decreased. The change in

where is the thickness of the surface sublayer, s is the density of sucrose crystal, C is the bulk concentration, Ci is the solute concentration at crystalsolution interface, and DAB is the mutual diffusion coefficients in watersucrose system, which is a function of solution temperature and concentration. Eq. (2) includes two terms that depend on the solution concentration. The diffusion coefficient, DAB, decreases with concentration, while the supersaturation (CCi) increases

a)

b)

c)

Fig. 2. Illustration of the way growth was modeled in a discrete matrix of volume element (in the xz plane). (a) Seed is placed in a center of volume element. (b) When the volume of the seed reaches the element volume, growth continued in the adjacent element. (c) Growth rates are function of the conditions in each volume element, therefore some faces grow faster than others. In this case the face in the top of crystal grew faster, therefore growth continued in adjacent elements around this face.

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Fig. 3. Predicted and experimental growth rates (m/min) of sucrose crystals during drying of thin sucrose films on microscope slides in different drying temperatures as function of air relative humidity (left chart) and initial film concentration (right chart). The lines represent the predicted results, and the marks with the error bars the experimental results (data from Howell and Hartel, 2001).

concentration was calculated from a mass balance on sucrose and water. 2) Generation of fusion heat: Crystal growth generated heat that raised the candy temperature. A term was added to the heat transfer equation, relative to the mass that was built on the crystal. 3) Decrease in diffusivity: The volume of a crystal acted as a barrier for diffusion of sucrose and water. To model this influence, a mass transfer of zero was used between two points when a crystal was present between them. 4) Decrease in drying rate: Crystals that grew on the surface decreased the surface area for water migration from the

solution to the air. In order to take this into account, the drying surface area was multiplied by one minus the ratio of crystal cross sectional area to solution cross sectional area in the direction of water flux. 2.4. Predicting the appearance The overall abundance of sugar crystal coating was determined in a visual descriptive sensory analysis by 33 panelists. The panelists were asked to indicate their assessment of the appearance, where 1 = sugar crystal coating not apparent (absent, coating looks clear as the solution is glassy) and 7 = extensive sugar crystal coating (extremely abundant, coating appears
100

%TS
100.0 99.5 99.0 98.5 98.0 97.5 97.0 96.5 96.0 95.5 95.0 94.5 94.0 93.5 93.0 92.5 92.0 91.5 91.0 90.5 90.0 89.5 89.0 88.5 88.0 8.3 41.7 57.6 75.0 108.3 141.7 8.2 175.0

98 96

92 90 88 86 84 82 80 100 90 110 120 88-90 96-98

50

X direction (m)

Distance from bottom (m)

Distance in film from bottom (m)

13

10

30

20

107.0

48

30

65

82-84 90-92

40

82

60

156.4

99

84-86 92-94

70

Drying time (sec)

80

86-88 94-96

Fig. 4. Concentration fields (in % total solids) around growing crystals after 115 s of drying of thin sugar film. Seed crystals were initially placed in 3 locations in film. Sucrose solution conditions: initial concentration 83% TS, temperature 71.0 C. Film thickness 103.8 m. Drying air conditions: temperature 80 C, velocity 1.0 m/s, relative humidity 10%.

Fig. 5. Sucrose solution (TS) concentration vs. time and location during drying of thin sugar film with initial dense layer of seed crystals 48 m from bottom. Sucrose solution conditions: initial concentration 83% TS, temperature 71.0 C. Film thickness 103.8 m. Drying air conditions: temperature 80C, velocity 1.0 m/s, relative humidity 10%.

% TS of sucrose

94

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229

Fig. 6. Simulation of temperature during drying of thin sucrose film of 104 m thickness with dense crystal seeding. Air temperature was 80 C, velocity of 1 m/s, and relative humidity of 25%. Initial film concentration was 83% TS.

white, as most sugar is crystallized). The crystal area coverage, A, was correlated to the film crystallinity, x, to get Eq. (3): A 3:8912x2 9:0155x 1 R2 0:9285 3

This correlation was combined into the model. Since the model predicted the crystallinity of the coating, using Eq. (3) it can determine the appearance of the coating. 3. Results 3.1. Simulating the effect of process conditions on crystallization rate The program was used to determine growth rate of sucrose in thin films under various process conditions. Results were compared to experimental work conducted by Howell and Hartel (2001). In general, good agreement between predicted and experimental results was achieved. Both experimental and simulated results showed the significant impact of temperature and relative humidity on growth rate and the minor impact of air velocity and initial film concentration (Fig. 3).

The growth rate increased substantially with air temperature. Above 40 C volume diffusion governs sucrose crystal growth rates and as the temperature increased, the diffusivity of sucrose molecules was higher and the growth rate increased. On the other hand, increasing the temperature decreased the supersaturation due to lower solubility, which would tend to inhibit growth. However, in this case, temperature elevation also increased the drying rate and the concentration in the film, so a decrease in supersaturation was not obtained. Air velocity had almost no effect on crystal growth because it had no effect on drying rate (under the simulated conditions internal water diffusion determined the drying rate) and had no effect on the internal conditions in the film. Relative humidity of the air directly affected the film concentration. When the air was moist (4050% RH) the film concentration was low (80%), resulting in lower supersaturation and slower growth. When the air was very dry, the film concentration became so high that the decrease in mobility inhibited crystal growth. At the optimal 35% RH the film concentration was approximately 90%, which gave maximum growth rate at 80 C. Initial concentration in the range of 75% to 85% had only a minor effect on crystal growth. Observing the concentration profiles in the film in the simulation output gave an explanation: drying occurred so

Table 2 Process conditions for intense drying of sugar-coated substrate (process A), and the simulation results Stage Description Process conditions Time (min) 1 Transport to dryer 0.2 Air temperature (C) 26 Air velocity (m/s) 0.11 Air humidity (g w/g da) 0.009 (40% RH) Results (end of stage) Sugar coating phase state 99% solution (81% TS) 1% crystalline No glassy material 44% solution (99% TS) 56% crystalline No glassy material 0% solution 59% crystalline 41% glass at 96.4% TS Crystal area coverage 1.06 Tg (C) 41.6 aw 67%

Drying

4.0

80

1.0

0.003 (1.5% RH)

4.81

44.8

0.3%

Cooling

2.0

21

1.0

0.004 (30% RH)

4.97

29.7

5%

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Table 3 Process conditions for optimized drying of sugar-coated substrate (process B) and the simulation results Stage Description Process conditions Time (min) 1 Transport to dryer 0.2 Air temperature (C) 26 Air velocity (m/s) 0.11 Air humidity (g w/g da) 0.009 (40% RH) Results (end of stage) Sugar coating phase state (end of stage) 99% solution (81% TS) 1% crystalline No glassy material 91% solution (95% TS) 9% crystalline No glassy material 3% solution (94% TS) 97% crystalline No glassy material 1% solution (95% TS) 99% crystalline No glassy material Crystal area coverage 1.06 Tg (C) 41.6 aw 66%

Intense short drying

1.0

80

1.0

0.003 (1.5% RH)

1.78

24.9

9.2%

Mild long drying

3.0

80

1.0

0.046 (15% RH)

6.09

17.7

14%

Cooling

2.0

26

1.0

0.08 (30% RH)

6.12

23.6

10%

rapidly that the solution approached high supersaturation very quickly regardless of initial concentration. 3.2. Growth velocity of the crystals faces and concentration fields A simulation of growth of three 10 m seed crystals, that were virtually placed in a sugar film, was performed in order to follow the change of crystal size and shape and the concentration fields. The crystal faces grew at rates proportional to their respective surface concentration. At initial stages of drying, when the film concentration was at its lowest, the crystal faces that were closer to the air interface grew faster since the concentration at the surface was higher. Later, when the film concentration was high and molecular mobility restricted growth, the face closer to the bottom of the film grew faster since the concentration at that surface was now lower. The concentration below the crystals was low compared with other regions in the same horizontal layers due to a combination of growth desaturation and the crystals acting as a barrier for moisture migration upward (Fig. 4). Fig. 5 describes the concentration in a sucrose solution when a dense layer of seeds was placed in a horizontal layer in the center of the film. Simulation showed that the crystals grew in all directions, forming a crystalline layer between two liquid layers. Initially, the concentration at the bottom of the film increased because of the drying; but after 40 s, once a closed solid layer of crystals had formed, the concentration near the bottom of the film decreased because the solid layer blocked the water movement upward and sugar was removed from solution during growth. 3.3. Appearance of coating For a given seed density and location, the drying conditions had the same effect on the crystal area coverage as on growth rate (Section 4.1). An initial high density of seeds in the film led to more crystal growth and resulted in more crystalline material. Therefore, dense seeding is an advantage in order to

get maximum crystalline appearance. The simulation results showed that the best location for seeds, in order to maximize crystal growth, was at the bottom of the film. During drying of thin films, the film concentration closer to the surface increased above the optimal concentration for growth and inhibited crystallization. At the bottom of the film, the concentration was the lowest and was closer to the optimal concentration for growth. Therefore, the growth rate was faster at the bottom. Also, when seeds are located at the bottom of the film, a larger layer of crystalline material that inhibits further drying of the film was not formed. 3.4. Temperature of the sugar film Four factors affect the temperature of the sugar film during drying: the amount of heat absorbed from the air, the amount of latent heat released by water evaporation, the amount of heat that is generated by the growing crystals, and the thermal properties of the sugar solution. Fig. 6 shows the temperature change during simulation of drying and dense film seeding. An initial decrease of 4 C occurred because of evaporative cooling. After 20 s, the film temperature increased mostly by the heat absorbed from the drying air and partly by the heat generated during growth. After 70 s of drying, the temperature of the film increased above the drying temperature (due to the release of latent heat) and reached 81 C.
Table 4 Conditions for simulating storage of Cotton candy Conditions Initial candy temperature Initial candy floss thickness Initial sugar concentration Storage air temperature Storage air humidity Storage air velocity Exposure to medium air humidity 21 C 1 mm 99.9% TS 21 C 45% RH 0.1 m/s Exposure to high temperature 21 C 1 mm 99.9% TS 82 C 0% RH 0.1 m/s

In both cases we assumed that the air is moving past the candy at a speed of 0.1 m/s.

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231

100 98 96 94

0 92 20 90 40 88 60 86 84 82 21 63 100 146 229 80

Duration (min.)

Center

313

120 396 479

Distance in thread from center (m)

Surface

Fig. 7. Predicted sugar concentration profile in a Cotton candy exposed to air with 45% relative humidity. Initial sugar concentration was 99.9%.

3.5. Prediction of crystal area coverage and storage stability of sugar-coated substrate Two drying processes of sugar-coated substrate at 80 C were simulated. Both processes started with applying warm aqueous sugar solution over substrate in a thin film and seeding. The main difference between the processes was that process (A) included intense drying, while process (B) included drying in 2 steps, optimized to achieve highest crystal growth rate. Drying conditions for process B were chosen in the following way: Based on Eq. (2), maximum growth rate at 80 C is
80 70 60

achieved at 94%. Process (B) included step of fast drying to reach this concentration, and a longer step of mild drying to maintain this concentration, while the crystals grew. The 94% concentration was controlled by the humidity of the drying air. The Norrish equation (Norrish, 1966) gives the equilibrium film concentration for a given relative humidity of the surrounding air. To achieve a concentration of 94%, the relative humidity of the drying air was adjusted to 15.4%. The process conditions and simulation results are described in Tables 2 and 3. While conveying the product at room temperature (step 1), the films were cooled and the seed crystals started to grow. The drying duration was 4 min in both processes (step 2), but process B gave higher crystallinity (97% compared to 56%), and higher crystal coverage area because of its optimal conditions for growth. In addition the film in process A reached higher concentration (98.8% TS), which correspond to high Tg (44.8 C). When drying process ended, film A cooled below this temperature, it became glassy and no more crystal growth occurred. Film B had lower concentration, lower Tg, and did not become glassy. At the end of the process (step 3), film B was in a more stable condition for storage: 99% was crystallized, compared to film A where only 59% was crystallized, and the remaining solution had aw of 5% and Tg of 29.7 C. With this low water activity, film A would probably pick up moisture from the air and become sticky. Even if it was wrapped with a moisture barrier, at temperatures above 29.7 C its glassy structure would collapse and it would start to crystallize. 3.6. Simulation of cotton candy storage Cotton candy is an amorphous sugar that is very prone to moisture sorption and high storage temperatures. To make cotton candy, sugar is heated to a point above the melting temperature (190 C) in a spinning head. The melted sugar is forced through tiny holes into a bowl that catches the candy floss. The fast cooling of the floss ensures that the sugar is amorphous.
20 10

% TS of sucrose

Unsaturated Solution

Temperature (C)

50 40 30 240 20 10 0 60 65 70 75 80 85 90 95 120 60

Supersaturated Solution

3 2 1

Solubility Curve

Glass Transition Curve

Glass
100

Sucrose Concentration (% Total Solids)

Fig. 8. Phase diagram for watersucrose system. The dotted line on the chart represents the predicted average sugar concentration of a Cotton candy exposed to medium air humidity. The dashed line represents the predicted temperature change of a Cotton candy exposed to high temperature. The numbers on the line represent the time duration in minutes to get to that point.

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Simulations of cotton candy storage were done under 2 environmental conditions: exposure of candy to medium air humidity (45%) at room temperature, and exposure of candy to high temperature (82 C) without moisture transfer. The simulation conditions are detailed in Table 4. 3.6.1. Exposure to medium air humidity Fig. 7 shows the reduction in sugar concentration when cotton candy was exposed to air at 45% RH. The surface of the amorphous sugar absorbed water rapidly, until reaching the equilibrium concentration of 88% TS. The sugar and water mobility increased, and water penetrated toward the center of the floss. After 4 h, the entire floss was at concentration below 90% TS. Fig. 8 shows the sucrosewater phase diagram, and the dashed line represents the change in the concentration of the candy. When the concentration of the candy decreased to below 94.6% (Cg at 21 C) the sugar started to crystallize. This happened after approximately 70 min. Simulation showed that after 2 h the majority of the floss had crystallized and the amorphous structure collapsed. 3.6.2. Exposure to high air temperature After exposure of the floss to high temperature, it took approximately 20 min for the candy to reach 82 C (Fig. 8, dotted line). However, the candy reached the glass transition point of 62 C quickly, to become a sugar melt. As the mobility of the sugar molecules increased with viscosity increase, the sugar started to crystallize. The crystal growth rate at 82 C is predicted by Eq. (2) approximately 90 m/min. 4. Summary A model to predict the concentration profile and growth of sugar crystals in a thin film has been developed and utilized to study various conditions of sucrose crystal growth. The model solves the unsteady state mass transfer equation coupled with an appropriate growth kinetic model to predict crystal size during drying of a thin film of sucrose with seed crystals imbedded in the film. By coupling this model with sensory measurements of film appearance based on area of crystal coverage, the crystal area coverage, as related to sensory

appearance, can be modeled for different operating and storage conditions. Acknowledgments Financial support for this study was provided by Kellogg's Company. The authors would like to express their gratitude to Mr. David Howlling and Mr. Terry Howell for their assistance. References
Ben-Yoseph, E., Hartel, R. W., & Howling, D. (2000). Three-dimensional model of phase transition of thin sucrose films during drying. Journal of Food Engineering, 44, 1322. Felder, R. M., & Rousseau, R. W. (1986). Elementary principles of chemical processes. Wiley Series in Chemical Engineering, 2nd Edition. New York: John Wiley and Son. Geankoplis, C. J. (1983). Transport processes and unit operations, 2nd Edition. Boston: Allyn and Bacon Inc. Hartel, R. W. (2001). Crystallization in foods. New York: Aspen. Honig, P. (1953). Principles of sugar technology. New York: Elsevier Publishing Company. Howell, T. A., Ben-Yoseph, E., Rao, C., & Hartel, R. W. (2002). Sucrose crystallization kinetics in thin films at elevated temperatures and supersaturations. Crystal Growth and Design, 2(1), 6772. Howell Jr., T. A., & Hartel, R. W. (2001). Drying and crystallization of sucrose solutions in thin films at elevated temperatures. Journal of Food Science, 66 (7), 979984. McCabe, W. L., Smith, J. C., & Harriot, P. (1985). Unit operations of chemical engineering, 4th Edition. New York: McGraw-Hill. Norrish, R. S. (1966). An equilibrium for the activity coefficients and equilibrium relative humilities of water in confectionery syrups. Journal of Food Technology, 1, 2539. Pancoast, H. M., & Junk, R. W. (1980). Handbook of sugars, 2nd Edition. Connecticut: The Avi Publishing Company. Perry, R. H., & Chilton, C. H. (1973). Chemical engineers handbook, 5th Edition. New York: McGraw-Hill. Reiser, P., Birch, G. G., & Mathlouthi, M. (1995). Physical properties. In SucroseProperties and Application. London: Blackie Academic and Professional. Roos, Y., & Karel, M. (1991). Applying state diagrams to food processing and development. Food Technology, 45, 6671. Wey, J. S. (1981). Basic crystallization processes in silver halide precipitation. In W. R. Wilcox (Ed.), Preparation and Properties of Solid State Materials, Vol. 6. (pp. ). NY, New York: Marcel Dekker, Inc.