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Journal of Food Engineering 46 (2000) 277285

www.elsevier.com/locate/jfoodeng

Freezing and ice crystals formed in a cylindrical food model: part I.


Freezing at atmospheric pressure
D. Chevalier a, A. Le Bail a,*, M. Ghoul b
a

Laboratoire de G
enie des Proc
ed
es Alimentaires, ENITIAA, Rue de la G
eraudi
ere, BP 82 225, F-44322 Nantes Cedex 3, France
b
ENSAIA, 2 Avenue de la for^
et de Haye, F-54500 Vandoeuvre les Nancy, France
Received 13 January 2000; accepted 30 May 2000

Abstract
Cylindrical gelatin gels were frozen at atmospheric pressure with dierent operating conditions (air-blast freezing at dierent air
temperatures and brine freezing). A method to calculate a local freezing rate was proposed to take into account the variation of
freezing rate as a function of the radius. A linear evolution of the local freezing rate according to the radius was observed whatever
the freezing process was. Frozen gels were freeze-dried and sliced perpendicularly to the heat ux. The ice crystal marks were
measured according to the radial position with image analysis software. Each radial distribution of ice crystal size was characterised
by the mean representative diameter. A linear regression permitted to link the ice crystal mean representative diameter to the radial
position. On addition, the variation in the mean diameter with the local freezing rate was tted by a power law. 2000 Elsevier
Science Ltd. All rights reserved.
Keywords: Freezing; Ice crystal size; Gelatin gel; Cylindrical geometry

1. Introduction
Freezing is an ecient preservation process because
of the transformation of liquid water into ice which reduces greatly microbial and enzymatic activities. But ice
crystals formed during freezing have a great inuence on
the quality of foodstus after thawing causing drip
losses, textural and colour modications (Fellows,
1988). The size of ice crystals in a frozen sample depends
on the number of nuclei formed during freezing. Ice
nucleation is mainly initiated during the rst-degree fall
below the initial freezing temperature. Thus, it is important to control the operating conditions during this
phase to obtain good nucleation. It is well known that a
fast freezing rate tends to form a ne ice structure which
causes less damage to the structure of the product while
a slow freezing rate leads to large ice crystals (Reid,
1993). Although the relation between ice structure and
freezing rate in food have been mostly qualitative (Bello,
Luft, & Pigott, 1992; Grujic, Retrovic, Pikula, &
Amidzic, 1993), some studies have quantitatively related

ice crystal size to freezing rate. These latter studies,


summarised on Table 1, have used samples insulated on
all sides except one where heat exchange takes place to
ensure one dimensional heat transfer (slab geometry).
Faced with various denitions of the freezing rate it is of
importance to dene this term more accurately. The
freezing rate is most of the time used to compare
freezing techniques (i.e. cryogenic vs air-blast). In the
literature, freezing rate is numerically represented in two
ways. The rst one is the approach of Plank (1941) who
dened the freezing rate as the velocity of the phase
change front ([dimension]/[time]). It is based on the
linear velocity of the phase change front called LVA in
the rest of this paper. Plank equation to estimate the
freezing time is given by Eq. (1), M and N being coefcients corresponding to slab and cylindrical geometry
as indicated in Table 2. The inverse of the derivative of
Eq. (1) yields the expression for the velocity of the phase
change front given in Eq. (2) for slab geometry and in
Eq. (3) for a cylindrical geometry.


DH q M
1 M

;
1
tc
Ta Tf N h 4k

Corresponding author. Tel.: +33-251-78-54-73; fax: +33-251-78-5467.


E-mail address: lebail@enitiaa-nantes.fr (A. Le Bail).

wx

0260-8774/00/$ - see front matter 2000 Elsevier Science Ltd. All rights reserved.
PII: S 0 2 6 0 - 8 7 7 4 ( 0 0 ) 0 0 0 8 9 - 3

Ta Tf
;
qDH 1=h x=k

278

D. Chevalier et al. / Journal of Food Engineering 46 (2000) 277285

Notation
coecient (m2 s1 )
coecient
representative ice crystal diameter (m)
mean representative ice crystal diameter (m)
maximum vertical distance between the cumulative distribution function of two samples in the KolmogorovSmirnov test
mass diusivity of water (m2 s1 )
temperature gradient in the j zone (C m1 )
heat transfer coecient (W m2 K1 )
enthalpy (J kg1 )
dendritic spacing (m)
characteristic dimension in Plank equation (m)
constant in Plank equation
radius (m)

a
b
dp
dp
Dobs
D
Gj
H
H
L
M
N
R

r0
R
tc
T
Ta
Tf
U
W
x

external radius of the cylinder (m)


overall freezing front rate (m s1 )
freezing time (s)
temperature (C)
ambient temperature (C)
initial freezing temperature (C)
local freezing rate (m s1 )
freezing rate from Plank equation (m s1 )
cartesian coordinate of a slab (m)

Greeks
k
thermal conductivity of the frozen food (W m1 K1 )
q
density of frozen sample (kg m3 )
Subscripts
1
frozen zone
2
unfrozen zone

Table 1
Characterisation of mean crystal size (technique of observation, range of size) in relation with freezing rate for slab geometry
Product

Freezing rate

Observation
technique

Alloys

Beef

Relation with
freezing rate

Reference

4060

dp / RG2

Freeze-substitution

1045

dp / 1=RG2

5200

dp / Rb

Tiller and Rutter


(1956)
Bevilacqua et al.
(1979)
Reid (1980)

5500

L  dp / 1=RG1 0:5

50500

dp / D=R

Sucrose
solutions
Apple tissue

0.031C/min450C/min

Protein gels

0.0030.02 m/h

Cryo-scanning
electron microscopy
Cryo-scanning
electron microscopy
Freeze-xation

Gelatin gels

Freeze-drying

10100

L  dp / 1=RG1 0:5

Gelatin gels
with salt

Freeze-drying

50700

L  dp / 1=RG1 0:5

wr

1.25C/min100C/min

Mean size
observed (lm)

Ta Tf
;
qDH r=r0 h r=kLnr0 =r

On the other hand, the International Institute of


Refrigeration (1986) dened the nominal freezing time
as the duration between 0C and 10C below the initial
freezing temperature at the thermal centre. Based on this
latter approach, most researchers calculated the freezing
rate as the ratio of temperature dierence and the respective duration ([K]/[time]). This method considering
the cooling velocity during phase change is called CVA
Table 2
Coecients M and N for Plank equation (Eq. (1)) according to
geometry
Geometry

Innite slab
Innite cylinder

Thickness
Diameter

2
4

Bomben and King


(1982)
Miyawaki et al.
(1992)
Woinet et al.
(1998b)
Woinet et al.
(1998b)

in the rest of the paper. In this case, a starting criterion


and an ending criterion for freezing must be dened. Le
Bail and Cornier (1994) showed that this freezing rate is
not dependent of the temperature history during freezing (if the same temperature dierence and the same
duration is considered). From Ramaswamy and Tung
(1984), the eective freezing time appears to be the more
acceptable denition of freezing time. The eective
freezing time is dened as the total time required to
lower the temperature of the product from its initial
value to a given temperature at the thermal centre (International Institute of Refrigeration, 1986). Freezing
rate was dened from this time as the ratio between the
minimum distance from the surface to the thermal
centre, and the time elapsed between the surface reaching 0C and the thermal centre reaching 10C lower than
the temperature of initial ice formation at the thermal
centre.
Researches on slab geometry were interested in
relations between representative ice crystal size and

D. Chevalier et al. / Journal of Food Engineering 46 (2000) 277285

location, freezing time or freezing rate. For example,


Bevilacqua, Zaritzky, and Calvelo (1979) did histological studies on beef pieces (5 cm in diameter and 10 cm in
length) frozen under controlled conditions. They observed a linear relation between the average diameter of
ice crystals and the logarithm of the characteristic
freezing time dened by these same authors. They also
correlated the extracellular ice crystal size with the linear
velocity of the freezing front according to the theory of
Tiller and Rutter (1956). They obtained a relation
linking the average diameter of ice crystal to the inverse
of the speed of the freezing front (LVA) and the temperature gradient at the phase change front (Table 1).
Bomben and King (1982) studied ice morphology in
frozen apple tissue (2 cm in diameter and 3 mm thick)
according to the CVA freezing rate. They measured
dendritic spacing as a function of the CVA freezing rate
and showed that dendritic spacing was proportional to
the inverse square root of CVA freezing rate. They were
the rst to apply the constitutional supercooling theory
to food. This theory was developed in the eld of metallurgy (alloys) and solutions domains. Rohatgi and
Adams (1967a,b) calculated dendritic spacing using
constitutional supercooling conditions which resulted in
the maximum solute concentration dierence in the interdendritic zone. A model to describe the mean size of
ice crystal was proposed too by Miyawaki, Abe, and
Yano (1992). These authors observed that the product
of the representative ice crystal size and the LVA
freezing rate was proportional to the diusion coecient
of water (Table 1). They successfully applied this relation in the case of freezing of protein gels (soy protein
and egg albumin gel). Woinet, Andrieu, Laurent, and
Min (1998b) recently determined ice crystal distribution
in frozen gelatin gel for many operating conditions with
and without sodium chloride salt. A model based on the
principle of the supercooling resulting from the maximum concentration dierence in the interdendritic zone
was proposed to interpret experimental relationships.
For the determination of freezing rate dierent approaches have been used. Bevilacqua et al. (1979) exploited experimental data based on the LVA approach
and the temperature gradient according to position in
samples as in Woinet, Andrieu, and Laurent (1998a) and
Woinet et al. (1998b). Bomben and King (1982) expressed
the moving speed of the freezing front based on an
analytical model of freezing (Plank model). A more complex method (three-step model) was used by Miyawaki
et al. (1992) to evaluate the temperature of the sample
during freezing and the velocity of the freezing front.
Various methods have been used to measure the ice
crystal size as shown in Table 1. Direct methods such as
cold stage scanning electron microscope (Reid, 1980,
Bomben & King, 1982) are interesting to observe ice
crystals, as the frozen sample is not aected by chemical
or physical changes. Nevertheless, this technique re-

279

mains expensive and time-consuming and is not suited


to study of numerous samples. Indirect methods such as
freeze substitution, freeze xation and freeze-drying
techniques have the disadvantage of requiring processing steps to prepare samples before observation and
might therefore introduce artefacts. Freeze substitution
consists of replacing ice by a solvent (methanol for example), evaporating it and observing the sample directly
or after embedding (Bevilacqua et al., 1979). The freeze
xed samples is immersed into xative solution (glutaraldehyde) which migrates into the sample and creates
links between proteins to x the sample structure
(Miyawaki et al., 1992). The freeze-drying has the advantage of being easy to carry out and gives satisfactory
results (Kochs, K
orber, Heschel, & Nunner, 1993).
The singularity of this work lies in that it concerns
freezing of cylindrical geometry cooled in the radial direction. The model food chosen is gelatin gel because
of its homogeneity and ease of reproducibility of its
structure. Such characteristics could not be ensured with
real foodstus, which have a great variability in structure, texture and composition. Besides this similar
model food was successfully used by Woinet et al.
(1998a,b) to observe ice crystal. The objective of this
paper is to compare dierent freezing methods: air-blast
freezing at selected air temperature and brine freezing on
the rate of ice crystal formation. The determination of
crystal size distributions according to the radial position
is carried out to evaluate the inuence of the radial location on ice crystal distributions. Secondly, relationships between the mean ice crystal size, the location and
the velocity of the phase change front are studied.
2. Material and methods
2.1. Model material preparation
To prepare 2% (w/w) gelatin gels, powdered gelatin
(Merck, Darmstadt, Germany) was dissolved in distilled
water and placed in an hermetic ask. The solution was
mixed for 1 h at 20C at 100 rpm min1 with a magnetic
stirrer. The mixture was then heated for 30 min at 50C
at the same stirring rate. After cooling to 40C, this
mixture was poured into cylindrical plastic lms (Betan,
Soussana SA, Thiais, France), 0.1 mm wall thickness,
40 mm in diameter and 200 mm in length. The gelation
process was achieved after 12 h at 5C. This preparation
stage is necessary to reach gel maturity and to obtain for
each preparation the same gel structure and texture
(Woinet et al., 1998a).
2.2. Freezing processes
Gels were frozen either in an air-blast freezer (Servathin, France) or in a brine freezer. Two dierent

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D. Chevalier et al. / Journal of Food Engineering 46 (2000) 277285

Fig. 1. Experimental cylindrical gel: size, thermocouples locations and presentation of the method to calculate the local freezing rate.

ambient air temperatures )20C and )30C were used in


the air-blast freezer with an air speed of 4 m s1 . Brine
freezing was carried out at )20C in a stirred brine bath
of 50% (v/v) aqueous solution of ethylene glycol (Glacelf, Elf, France). The bath volume was 0.12 m3 . Initial
temperature before freezing was uniform and constant
(5C) in the whole sample. Two samples were frozen
together for each freezing conditions: one was intended
to be freeze-dried and the other was tted with six
chromelalumel thermocouples (0.3 mm diameter,
Omega, USA) placed at selected radial locations (Fig.
1). Temperature accuracy was 0.1C after calibration
from Pt 100 reference thermal probe (Allemand, Lyon,
France). Temperature changes during freezing were recorded using a data logger (AOIP, France). After
freezing this second sample was partially thawed. The
location of each thermocouple was then veried after
freezing by removing the gel close to the sensors.
2.3. Ice crystal size determination
As soon as samples were completely frozen, they were
freeze-dried. Freeze-drying was accomplished using a
condenser temperature of )86C and a vacuum pressure
of 2.7 Pa. Care was taken in controlling the temperature
of the samples during freeze-drying to avoid ice melting
and structured collapse. The ask in which the sample
was held, was maintained at 5C for seven days and the
temperature was increased to room temperature over
three days in steps of 5C. It was assumed that the
sublimated ice crystals left pores with minimal deformation and that these pores had the same size as the ice
crystals. This assumption of minimal deformation is
done in keeping in mind that it rejected to take into
account an intensive vapour ow through a matrix with
very thin walls. The middle part of the freeze-dried
sample was selected as shown in Fig. 1 assuming one
dimensional heat transfer in this part of sample. Thin
slices were cut perpendicularly to the heat ux with a
thin razor blade. Each slide was observed with a stereomiscroscope (Wild M3C, Leica Microsystems, Germany) tted with a CCD RGB camera (MACC-C71,

Sony, Japan) which records black and white images.


Images had 256 grey levels with a resolution of
512  512 pixels. Each image was treated with an image
analysis software (Visilog 4.1.5, Noesis, France), which
carried out numeric (contrast and threshold steps) and
morphologic treatments. Surface and perimeter of pores
were evaluated after calibration and the minor diameter
dp (representative diameter) of the ovoid section
considered was calculated (Bevilacqua et al., 1979;
Miyawaki et al., 1992). Each radial position was characterised by around 300 pores to obtain the corresponding ice crystal diameter distribution. For each
radial location, the relative cumulative distribution was
evaluated with respect to the representative diameter of
the ice crystals.
2.4. Statistical analysis
For each freezing condition, three samples were frozen and analysed. The two-sample KolmogorovSmirnov test (Daniel, 1990) was carried out to compare pairs
of relative cumulative distributions of ice crystal size and
to evaluate whether they were statistically dierent. This
test is used to test the null hypothesis that two independent samples taken from two dierent populations
are identical with respect to location and dispersion. The
test calculates the maximum vertical distance Dobs between the cumulative distribution function of the two
samples. If this distance is large enough, the hypothesis
that the two samples come from the same distribution is
rejected with a 95% condence level.
3. Results and discussion
3.1. Analysis of thermogramms
The temperature history distributions were recorded
for each freezing condition. An experimental temperature prole obtained for air-blast freezing at )20C air
temperature is presented with the exact location of
thermocouples in Fig. 2. Freezing can be divided in three

D. Chevalier et al. / Journal of Food Engineering 46 (2000) 277285

281

Fig. 2. Temperature proles during air-blast freezing with an air temperature of )20C and an air speed of 4 m s1 . Arrows indicate the radial
locations (mm) of thermocouples.

steps: initial refrigeration without freezing (precooling),


a plateau corresponding to the crystallisation zone
(phase change) and nally the tempering step. The 2%
(w/w) gelatin gel freezes at a constant temperature of
)0.3C. The freezing depression could be due to the
presence of a small amount of protein and to a slight
freeze-concentration eect. The freezing rate was evaluated according to the denition proposed by Ramaswamy and Tung (1984) based on the eective
freezing time (International Institute of Refrigeration,
1986). This mean freezing rate was obtained from the
ratio of the radius of the sample to the freezing time.
The freezing time was considered as the duration between the initial time for which the rst point of the
product reaching 0C and the nal time for which the
temperature of the centre of the product is 10C below
the initial freezing temperature. In our case the eective
freezing rates were 1:1  105 , 7:5  106 and 5:2  106
m s1 , respectively, for brine freezing, air-blast freezing
at )30C and air-blast at )20C. This method to calculate the freezing rate has been shown as a convenient
method if a relationship between the overall ice crystal
size and the freezing rate was searched (Ramaswamy &
Tung, 1984). But the freezing rate varies during the
process according to the considered location in the
sample leading to a freezing rate distribution. Therefore
this mean freezing rate does not bring enough information to describe the real nature of the freezing according to the location. Thus, a local freezing rate,
named u, was calculated from the experimental temperature proles shown in Fig. 1. The velocity of the
freezing front was evaluated from the ratio of the distance between two successive thermocouples (Dr) to the
freezing time dierence between these two locations (Dt).
The freezing time dierence was the time between the
end of the two freezing plateaus considered (Fig. 1).
Since the local freezing rate described above corresponded to an average freezing rate between two loca-

tions, this value was assigned to the geometrical centre


of the annular section bounded by the two locations.
The local freezing rates of the dierent freezing methods
are presented in Fig. 3 according to the radial position.
A linear regression was obtained between the local
freezing rate and the radial position for each freezing
condition with a strong correlation (R2 squared between
0.94 and 0.97). It appeared that the local freezing rate
increased linearly from the surface of the samples to the
centre. However the way of calculating the local freezing
rate did not permit evaluation very close to the centre
where it is expected to be innite according to the Plank
equation (Eq. (3)). Besides, a dierence was observed
close to the cooling surface for brine freezing sample.
The freezing rate increased slightly from the radius
12 mm due to the high heat exchange coecient of the
brine. The convective heat exchange prevailed in this
part of the sample. This variation is dierent from the
one observed in the case of slab geometry for which the
local freezing rate decreased from the surface to inner
location. An exception is the one observed at the surface
of the brine-frozen sample. Indeed, the heat ux to the
phase changes front decreases as the front travels into
the geometry. This is due to the increase of the thermal
resistance of the frozen part located between the

Fig. 3. Local freezing rate according to the radial position in a cylindrical 2% gelatin gel for air-blast freezing )20C (}), air-blast freezing
)30C (h) and brine freezing )20C (D).

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D. Chevalier et al. / Journal of Food Engineering 46 (2000) 277285

refrigerated surface and the phase change front. In the


case of the cylindrical geometry, even if the thermal
resistance increases while the thickness of ice formed,
the volume to freeze is more and more reduced as the
phase change front moves toward the centre. Thus, the
velocity of the phase change front increases while it
moves away the surface.
3.2. Ice crystal formed in frozen samples
Slices of freeze-dried samples were carefully taken
parallel to the heat ux (Fig. 4(a)). Direct observations
revealed ice ngers growing parallel to the heat ux
from the external surface toward the centre of the
sample. The slices taken perpendicular to the heat ux
(Fig. 4(b)) showed the arrangement of ice crystals (light
spot) in the dry matter matrix (dark spot). The wall
between the ice crystals was very thin due to the low dry
matter concentration of the gelatin gels.
3.3. Ice crystal size according to the radial position
The dierent relative cumulative distributions of the
representative diameter dp for air-blast freezing at )30C

and brine freezing at )20C processes are presented respectively in Figs. 5 and 6. Whatever the freezing
method was, the distribution was more and more dispersed with increasing radius. The relative cumulative
distributions of ice crystal size showed a decrease in the
size of ice crystal from the surface to the centre except
for the radius 18 mm. In the case of air-blast freezing
()20C and )30C), the relative cumulative distribution
of the surface (radius 18 mm) was smaller than the one
of the radius 14 mm. In the case of brine freezing
()20C), this relative cumulative distribution at radius
18 mm was smaller than those of the two next radii
(14 mm and 10 mm). This was probably due to the high
heat exchange between the cooling medium (air or brine)
and the surface of the sample at the beginning of freezing. For brine freezing this phenomenon is correlated
with the particular evolution of the local freezing rate at
the surface of the sample previously described. The
spread of ice crystal size with radius was much larger for
the air-blast freezing processes than for brine freezing.
A statistical analysis was carried out based on the two
samples KolmogorovSmirnov test to identify dierences between the dierent distributions in the same
sample. Results for each test are quoted for air-blast

Fig. 5. Relative cumulative distribution of ice crystal diameter for ve


radial positions in cylindrical 2% gelatin gel. Freezing process: air-blast
freezing at )20C.

Fig. 4. Sections of freeze-dried cylindrical 2% gelatin gel frozen by airblast with a cooling temperature of )30C: (a) sliced parallel to the
heat ux ( 6.4); (b) sliced perpendicular to the heat ux ( 80).

Fig. 6. Relative cumulative distribution of ice crystal diameter for ve


radial positions in cylindrical 2% gelatin gel. Freezing process: brine
freezing at )20C.

D. Chevalier et al. / Journal of Food Engineering 46 (2000) 277285


Table 3
Pairwise comparisons of air-blast freezing ()20C) radial distributions
by KolmogorovSmirnov tests. In each cell, the rst value is Dobs and
the second one (bold character) is the P-value

283

Table 5
Pairwise comparisons of brine freezing ()20C) radial distributions by
KolmogorovSmirnov tests. In each cell, the rst value is Dobs and the
second one (bold character) is the P-value

Radius (mm)

14 mm

10 mm

6 mm

2 mm

Radius (mm)

14 mm

10 mm

4 mm

2 mm

18

0.24
(<0.00)

0.15
(0.014)
0.37
(<0.00)

0.35
(<0.00)
0.69
(<0.00)
0.16
(<0.00)

0.61
(<0.00)
0.78
(<0.00)
0.43
(<0.00)
0.30
(<0.00)

18

0.13
(0.02)

0.10
(0.21)
0.11
(0.17)

0.21
(<0.00)
0.27
(<0.00)
0.28
(<0.00)

0.24
(<0.00)
0.34
(<0.00)
0.34
(<0.00)
0.09
(0.26)

14
10
6

Table 4
Pairwise comparisons of air-blast freezing ()30C) radial distributions
by KolmogorovSmirnov tests. In each cell, the rst value is Dobs and
the second one (bold character) is the P-value
Radius (mm)

14 mm

10 mm

6 mm

2 mm

18

0.34
(<0.00)

0.40
(<0.00)
0.32
(<0.00)

0.69
(<0.00)
0.60
(<0.00)
0.33
(<0.00)

0.83
(<0.00)
0.69
(<0.00)
0.43
(<0.00)
0.17
(0.03)

14
10
6

freezing ()20C) and ()30C) and for brine freezing,


respectively in the Tables 35. The comparisons by pairs
are characterised by the maximum dierence between
the two cumulative distributions considered Dobs and by
the P-value of the test. Each radial distribution is statistically dierent to all the others distributions for the
two air-blast freezing processes (Tables 3 and 4). That
shows a signicant variation of the ice crystal size with
respect to the radial position. For brine freezing (Table
5) three tests show a P-value higher than 5% which indicates that the considered two radial distributions are
identical. So the distribution for radius 10 mm is not
statistically dierent from those of radius 18 and 14 mm.
That could be explained by the local freezing rate of
brine freezing which is nearly constant from the surface
to the radius 10 mm and so causes the same nucleation
rate in this zone. Besides the distribution at radius 4 mm
and the one at radius 2 mm are statistically identical.
For brine freezing the ice crystal size seems to tend to a
limit size and does so faster than for air-blast freezing
methods. This aspect will be discussed again in the
analysis of the evolution of the mean representative
crystal size.
Each radial distribution was characterised by its
arithmetic mean dp . The variation of the mean representative diameter dp with the radius is presented in
Fig. 7. A linear relation between the mean diameter and

14
10
4

the radius between r 2 and 16 mm was observed


whatever the freezing process was. The slope of the regression and the correlation coecient (indicated in
brackets) were respectively, 4.50 (0.92), 2.13 (0.98) and
0.74 (0.95) for air-blast freezing at )20C, at )30C and
for brine freezing at )20C. This linear variation with
the radius was the inverse of the one observed in the case
of slab geometry (Woinet et al., 1998b). For the slab
geometry the mean ice crystals size increased with the
distance from the heat exchange surface. As the freezing
front moved away from this surface the velocity of the
freezing front decreased due to the thickness of ice
formed. Therefore, the nucleation rate decays while the
phase change front travelled through the medium
yielding larger and less numerous ice crystals. In the case
of cylindrical geometry, the freezing rate tends to increase from the external surface to the centre of the
sample. This is shown by the Plank expression (Eq. (3))
for the phase change front velocity and is due to the fact
that, in cylindrical geometry, the volume of a given
annular increment is decreasing with decreasing radius.
Therefore, the required energy for freezing a same space
increment is decreasing from surface to centre. This
trend was correlated to the decrease in the ice crystal
size. The slope of the linear regression varied according
to the freezing process: the faster the process was, the

Fig. 7. Ice crystal mean diameter evolution according to the radial


position in a cylindrical 2% gelatin gel for air-blast freezing )20C (}),
air-blast freezing )30C (h) and brine freezing )20C (D).

284

D. Chevalier et al. / Journal of Food Engineering 46 (2000) 277285

A local freezing rate has been dened to take into account the change in freezing rate according to the radial
location. This local freezing rate changes inversely to the
representative diameter as a function of the radius.
These conclusions are very dierent from those obtained
with unidirectional heat ow freezing obtained in a slab.

Acknowledgements

Fig. 8. Ice crystal mean diameter evolution according to the local


freezing rate in a cylindrical 2% gelatin gel. Experimental data: () and
t model (A).

lower the slope. The range of change in ice crystal size


depends on the process and particularly on the freezing
rate. It is less obvious to interpret the intercept of the
linear regression with the ordinate axis: the slowest
process should produce the smallest ice crystals at the
centre but experimentally it seems that there is a common size at the centre for all freezing conditions (35
lm). This minimal size may be a minimum critical size.
At the surface (r 18 mm) a stagnation of dp was observed as shown in Fig. 7 for every freezing method.
These points were not taken into account in the linear
tting because of this particular behaviour due to the
convective phenomenon at the surface of samples.
3.4. Ice crystal size according to the freezing rate
The evolution of the mean representative diameter of
ice crystals with the local freezing rate is plotted in Fig. 8
which was obtained by pooling all the results. A power
law was chosen to t the experimental data as proposed
by some other authors as Reid (1980). The t yields
Eq. (4) with R2 equal to 0.81.
dp a ub ;

with a 2.89 107 m2 s1 and b )0.45.


Reid (1980) proposed this relation for a sucrose solution without giving any value for a and b. This author
mentioned only that these two coecients were function
of sucrose concentration in the solution. Miyawaki et al.
(1992) set b equal to )1 and proposed that a was proportional to the diusion coecient of water for a soy
protein curd (8% of dry matter) which was contact
frozen (slab geometry).

4. Conclusion
As a conclusion the freezing of cylindrical gelatin gels
cooled on each face showed a decrease of the ice crystal
size with the increase in distance to the cooling medium.

Thanks to the French Ministry of Agriculture for nancial support (Ph. D. grant) and to Region Pays de
Loire and P^
ole Agronomique Ouest for supporting the
experimental cost. Thanks to Dr. H. S. Ramaswamy for
help in preparing the manuscript. Thanks to P. Cantoni
for technical support for image analysis.
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