DRYING TECHNOLOGY

Vol. 21, No. 2, pp. 249–263, 2003

Analysis of Heat and Mass Transfer

in Freeze Drying

Farial Jafar and Mohammed Farid*

Department of Chemical and Materials Engineering,

The University of Auckland, Auckland, New Zealand

ABSTRACT

The main objective of this work is to build a mathematical model

that describes heat and mass transfer in freeze-drying when both
plate heating and radiation heating are applied and also to provide
further understanding of the mechanism of the drying process. The
model, unlike other models, may be used for situations in which
sublimation occurs within a temperature range, i.e., the non-existence
of a sharp interface and also for cases in which more than one
interface may form. The developed model has been tested against
experimental measurements of freeze-drying of milk under different
operating conditions. Measurements were done using Virtis BT3.3ES
freeze dryer with vertical manifolds. The milk was contained in a
glassware, specially designed for this project. Four thermocouples

*Correspondence: Mohammed Farid, Department of Chemical and Materials

Engineering, The University of Auckland, Private Bag 92019, Auckland,
New Zealand; Fax: 649-3737463; E-mail: m.farid@auckland.ac.nz.

249

DOI: 10.1081/DRT-120017746 0737-3937 (Print); 1532-2300 (Online)

Copyright & 2003 by Marcel Dekker, Inc. www.dekker.com
250 Jafar and Farid

were fixed at different positions to track the drying progress. The

experimental measurements show no significant shrinkage in the
frozen milk when dried, leaving the milk highly porous in structure.
In this experimental work, the low thermal conductivity of the dried
layer was found to control the process without any significant mass
transfer resistance. This includes plate heating where drying was
found to progress from the heating surface similar to radiation
heating. This is unlike what has been reported in some of literature
that drying starts always from the top surface. The model, which was
based on heat transfer control, showed a reasonable agreement with
the experimental measurements of both plate heating and radiation
heating.

Key Words: Freeze-drying; Heat and mass transfer; Moving

boundary; Milk; Radiation and plate heating.

INTRODUCTION

Freeze-drying is a method of dehydrating frozen materials by a

process of sublimation under high vacuum. This drying method is
known for its ability to sustain food quality during the low temperature
drying due to the minimum loss of flavor and aroma, negligible shrinkage
and the absence of water, which minimize the chance of microbial
growth. The main drawback of the process from industrial point of
view, is the fact that it is very slow compared with other methods of
drying. Heat is supplied to the material either by conduction, radiation,
or both, but at a low rate to avoid local melting. Drying time in the
laboratory and industrial freeze dryers is of the order of several hours
compared with only few hours in some of the other types of drying.
The process may be successfully analyzed as a moving boundary analysis
where sublimation occurs at a retreating solid–vapor interface.
Most of the investigators have analyzed freeze drying based on the
radiation method of heating.[1,10,14,15,16] The heat, in this method is trans-
ferred through the dried crust and finally absorbed at the sublimation
interface. Two types of modeling approaches are found in the literature;
the most widely used one is the quasi-steady state model, which is based
on ignoring the sensible heat effect.[19,20] The other and less commonly
applied approach is that based on solving the transient heat conduction
equation in both frozen and dried regions.[5,8] Some investigators have
also solved the mass diffusion equation together with the heat conduction
equation in both phases.[20] However, it has been recognized, by most
of the workers that freeze-drying is a heat transfer controlled process
Heat and Mass Transfer in Freeze Drying 251

whenever radiation heating is applied. This is evident from the constant

sublimation temperature observed in all the reported freeze-drying
experiments, based on radiation heating. The internal mass transfer
resistance was measured[12] and found small compared to the internal
heat transfer resistance. This matter will be discussed further in this article.
It is the freeze-drying with plate heating, in which the literatures
show some contradicting conclusions regards the true mechanism of
drying. Most of the investigators have assumed that the drying occurs
from the non-heated surface of the material.[5,12,20] This implies that the
heat must be conducted through the frozen material before it will be
absorbed at the sublimation interface. Others[2] have stated that drying
occurs from the heating surface, suggesting that heat transfer through the
dried layer rather than frozen layer controls the drying process. It has
been reported[12] that both mechanisms of drying may occur, depending
on the nature of the materials, without providing further explanation.
In some of the reported experimental works on freeze-drying with plate
heating a non-constant sublimation temperature was reported,[11] while
others have reported a constant sublimation temperature during the
whole period of drying.[13,20]
Drying may occur from both sides, by applying plate heating and
radiation heating.[17] In such applications, the conventional moving
boundary analysis becomes more difficult to apply due to the formation
of two interfaces. The enthalpy or effective heat capacity method can be
applied to such a case. The method was developed for materials, which
undergoes phase change within a range of temperature such as frozen
meat.[3,18] However, it has been shown[6] that the method can be applied
even for pure materials that melt and solidify at fixed temperatures, by
assuming the phase change to occur within a narrow temperature range
of 2–4
C. The material was assumed to have an effective heat capacity,
which varies widely within this temperature range to account for the
latent heat of melting. The mathematical problem was simplified to
the solution of heat conduction with variable heat capacity within the
selected temperature range of melting. The same approach is applied
in this work to freeze-drying, which usually occurs at almost constant
sublimation temperature.
Microwave heating has been suggested as an effective means of
supplying heat to the materials in freeze-drying.[16,21,22] The main problem
in the application of microwave freeze-drying is the glow discharge, which
occurs at high vacuum. Heat is absorbed by the material at different
levels, depending on the location, water content, and microwave
frequency. The model developed in this work can be also applied to
such a case, whereas the simplified quasi-steady state analysis will fail.
252 Jafar and Farid

It is the objective of this article to present this new approach in the

calculation of heat and mass transfer in freeze-drying that can be used for
cases with difficult boundary conditions. The article will also provide
further understanding of the freeze-drying mechanism, based on the
information obtained from our experiments and those reported in the
literature. Most of the experimental measurements and theoretical
models developed in the literature for freeze-drying were concerned
with the time required for drying, which cannot be used to assess the
true mechanism of drying. In order to have full understanding of the
mechanism of heat and mass transfer in freeze-drying, temperature
distribution within the material must be measured with time. Such
measurements are available for radiation heating[15] but not widely
available for plate heating. Some investigators have limited their
measurements to the surface and center temperatures,[4] while most of
the others have measured weight loss or total drying time.

THEORETICAL ANALYSIS

Quasi-steady State Analysis for Radiation Heating

This analysis is based on the assumption that sensible heat of the

material is negligible compared with the latent heat of sublimation.
Simple calculations show that sensible heating does not account for
more than 4% of the total heating required. The analysis will be used
to assess the importance of external and internal heat and mass transfer
resistances, while the unsteady-state model, described later, will be used
to predict the experimental measurements of temperature distributions.
Heat is transferred by radiation from the heating source to the
material surface, followed by conduction through the low thermal
conductivity crust. The sublimation interface, which acts as a heat sink
is found to remain at a constant temperature. Water vapor flows through
the crust to the freeze-dryer condenser via the dryer chamber, experienc-
ing a significant pressure drop. Heat transfer rate is linked to the mass
transfer rate by the following equation:
Tr  Tsub Psub  Pc dY
¼ ¼ " ð1Þ
1=hr þ Y=kcr 1=km þ Y=cr dt
At the early stages of drying, the crust is not formed yet and Eq. (1)
simplifies to:
q ¼ hr ðTr  Tsub Þ ¼ km ðPsub  Pc Þ ð2Þ
Heat and Mass Transfer in Freeze Drying 253

Now since Tsub and Psub are related by the equilibrium ice vapor
pressure–temperature relationship, there will be a single value of Tsub
and Psub, which describes the system. If the sublimation temperature
remains constant then the drying rate will drop as time progresses, due
to the important contribution of the heat and mass transfer terms, as
shown by Eq. (1). In food, it is likely that the crust permeability is
proportional to its thermal conductivity, at a specific vacuum, causing
the mass and heat transfer resistances to increase in a similar fashion.
Integrating Eq. (1) gives the total drying time, which can be written
in term of either the heat or mass transfer parameters. Crust thermal
conductivity (kcr) and radiation heat transfer coefficient (hr) are easier
to measure than crust permeability () and external mass transfer coeffi-
cient (km). This explains why most of the investigators have related the
drying time to the external and internal heat transfer resistances. However,
it is not uncommon to find some calculations based on the internal mass
transfer resistance, while ignoring the external mass transfer resistance.[2]

Quasi-steady State Analysis for Plate Heating

As we have discussed earlier, two possibilities may occur during

freeze-drying with plate heating. One is based on the assumption that
drying may occur from the heating surface (Fig. 1A), where the heat
transfer rate may be expressed as follows:
Tp  Tsub dY
q¼ ¼ " ð3Þ
Y=kcr þ 1=hc dt
In this mechanism, the heat transfer through the crust controls the
drying process, as in radiation heating. The term 1/hc is known as the
contact thermal resistance between the heating plate and the tray contain-
ing the food. This contact resistance is a function of the vacuum applied

Figure 1. The two possible mechanisms of freeze-drying with plate heating.

254 Jafar and Farid

and the separation distance between the tray and heating plate.
The contact resistance was found to vary from 0.02 to 0.1 m2 s K/J.[9]
Equation (3) shows that drying rate will be initially high and is controlled
by the contact resistance. For example, the thermal resistance of 1 mm
thick crust is of the order of 0.02 m2 s K/J only. However, the dried crust
will grow and become the main thermal resistance as heating progresses.
Based on Eqs. (1) and (3), the plate temperature in the plate heating must
be kept at a temperature lower than that usually applied in radiation
heating, because the extra thermal contact resistance in the plate heating
is usually smaller than the radiation thermal resistance. This is in agree-
ment with the normal practice in plate heating, where the plate tempera-
ture is usually kept at about 40
C, compared with about 75–100
C in
radiation heating.[5,20]
In the other possible mechanism, the drying is assumed to occur from
the non-heated surface (Fig. 1B). Hence, heat must transfer through
the frozen layer to the sublimation interface where it is absorbed. The
generated vapor must flow through the crust formed and the heat and
mass transfer may be described by the following equation:

Tp  Tsub Psub  Pc dY
q¼ ¼ ¼ " ð4Þ
ððL  Y Þ=kice Þ þ 1=hc 1=km þ Y=cr dt

The conduction thermal resistance of the frozen layer will change

from about 0.02 m2 s K/J for 10 mm thick frozen layer to a very small
value as drying progresses. Hence the dominating thermal resistance will
be the contact resistance, which remains constant during the drying
process. If the sublimation temperature remains constant then the first
equality in Eq. (4) indicates that heat transfer will remain constant or
even increases due to the decrease of the frozen layer thickness (L Y ),
which is incorrect. In fact, the first equality in Eq. (4) cannot be true
unless the sublimation temperature increases as the crust thickness (Y )
increases, suggesting a mechanism of mass transfer control. This has not
been observed from the experimental work conducted here. Also, since
the thermal conductivity of ice is of the order of 20 times or more than
that of the dried crust[5] the temperature distribution within the frozen
material is expected to be small, which has been reported in the
literature.[4] The large difference between the plate temperature (40
C)
and the sublimation temperature (30
C) can be only due to the contact
resistance. The sublimation temperature was found to increase during
the drying process, confirming the mass transfer control mechanism.
Others have reported a constant sublimation temperature during the
whole period of drying.[13,15]
Heat and Mass Transfer in Freeze Drying 255

Transient Analysis of Freeze-Drying Using

the Effective Heat Capacity Method

The method illustrated in this section is based on the solution of the

unsteady-state heat conduction equation in one-dimension. The analysis
is based on heat transfer controlled drying, and includes the sensible
heat effect.
@T @2 T
¼ 2 ð5Þ
@t @y
y ¼ 0 T ¼ f ðtÞ as controlled by the plate heater ð6Þ
dT
y ¼ L  kcr ¼ hr ðTs  Tr Þ as controlled by the radiator ð7Þ
dx
In the plate heating experiment, most of the heat is received from the
heater located at the lower surface of the glass container, yet a small
amount of heat is conducted through the container wall and radiated
to the upper surface ( y ¼ L). In the radiation heating experiment, most
of the heat is received by radiation at the upper surface with small
amount conducted through the glass wall to the lower surface ( y ¼ 0).
Due to these effects, heat transfer near the glass wall will deviate from
one-dimensional.
The effective heat capacity or enthalpy method of solution is used
to solve the heat conduction equation with its boundary conditions. The
equation is solved in the frozen, dried, and sublimation regions, using the
corresponding physical properties of each phase. The sublimation is
assumed to occur within a specified temperature range. Physical properties
of the sublimation region are taken as the average of those of the frozen
and dried region. The latent heat is accounted for by using an effective
heat capacity (Cpe), which changes in the sublimation region according to
any selected function so that its integral is equal to the latent heat:
Z Tm2
ðCpe  Cps Þ dT ¼ w ð8Þ
Tm1

where w is the moisture content and  is the latent of sublimation of ice.

For pure materials, the maximum value of Cpe should be at the true
phase change temperature and phase transformation might be assumed
to occur within say 2
C. It has been shown[6] that the choice of the
function describing the variation of Cpe is not a critical, if the number
of space divisions selected in the finite difference calculation is reasonably
high to account for most of the latent heat effect. The method of analysis
has been recently applied[7] for the simulation of under floor heating.
256 Jafar and Farid

Phase-change material was used to increase the thermal mass of the

floor allowing more heat to be stored. Similar computational approach
has also been recently used to describe heat transfer during microwave
thawing of meat.[18]
The experimental apparatus described in the following section show
that plate heating has been applied from outside of the glass vessel
containing the frozen milk sample. The thermal mass and the conduction
resistance of the glass were not negligible and were included in the
analysis. Hence the application of Eq. (5) was extended to cover the
glass base and the boundary condition defined by Eq. (6) was applied
to the external surface of the glass rather than the frozen milk. The frozen
milk and the glass base of the vessel were divided into a number of space
divisions for the numerical solution based on finite difference method of
solution. In the computation, the time increment was automatically
selected, based on the stability requirements of the explicit finite differ-
ence method.

EXPERIMENTAL MEASUREMENTS AND THE

RESULTS OF SIMULATIONS

Powder milk was dissolved in water to make 30 wt% concentrated

milk. The milk was poured in the glass tray and frozen by dry ice down to
45
C. The tray was placed in the vacuum vial flask with the radiation
heater fixed at the top, and the plate heater fixed at the bottom as shown
in Fig. 2. Four thermocouples were fixed at locations 2, 9, 15, and 21 mm
from the bottom of the tray to measure continuously the temperatures
T1, T2, T3, and T4. The plate temperature (Tc) and radiator temperature
(Tr) were also measured. The total height of the frozen milk was 27 mm,
while all other dimensions are shown in Fig. 1.
The measured analogue signal from the thermocouples were
converted to digital signal by a Pico logger and sent to a PC for data
recording and processing. The plate and radiator heaters were connected
to a power supply with a variac to set the required heating power. Figure 3
shows the measured temperature at the different locations in the milk
sample, as drying progressed. Only part of the 6 W radiation heating
was received by the sample, while the remaining was dissipated from
the other side of the heater. Hence, the rated power was not used in
the simulation but rather the measured radiation heater temperature,
which was continuously increasing during the process. The sublimation
temperature remained constant during the whole experiment. The drying
progressed from the top to the bottom as expected with a total drying
Heat and Mass Transfer in Freeze Drying 257

Figure 2. Vacuum vial flask and the heating system.

Figure 3. Measured temperatures in freeze-drying of milk, using 6 W radiant

heating.

time of about 47 h. The predicted temperature variation at the same

locations is given in Fig. 4, which shows reasonable agreement with those
measured. Figures 5 and 6 present the measured and predicted tempera-
ture distribution for the same experiment. The observed differences
258 Jafar and Farid

Figure 4. Predicted temperatures in freeze-drying of milk, using 6 W radinat

heating.

Figure 5. Mesured temperature distrbution in freeze-drying of milk, using 6 W

radiant heating.

between the measured and predicted temperature distribution was mainly

due to the high degree of uncertainty in the physical properties of
the dried milk and in the calculated value of radiation heat transfer
coefficient.
The change in the measured temperature in the milk sample at
different locations using 2 W plate heating is shown in Fig. 7. The
measured heater temperature was used in the simulation and not the
rated power because small part of the heat supplied by the heater was
lost by conduction and radiation through the glass wall of the container.
Heat and Mass Transfer in Freeze Drying 259

Figure 6. Predicted temperature distrbution in freeze-drying of milk, using 6 W

radiant heat.

Figure 7. Measured temperatures in freeze-drying of milk, using 2 W plate

heating.

The sublimation temperature remained constant at 20
C during most of

the heating period. The results show that drying progresses from the
lower surface, which is close to the heater. The results shown in Figs. 9
and 10 also support the assumption that drying occurs from the heated
surface. The model predicted well the measured temperatures.

CONCLUSIONS

Measurements of temperature distribution during freeze drying of

milk were conducted in a one-dimensional arrangements. The results
260 Jafar and Farid

Figure 8. Predicted temperatures in freeze-drying of milk, using 2 W plate heating.

Figure 9. Measured temperature distribution in freeze-drying of milk, using 2 W

plate heating.

indicate that drying occurs from the material surface close to the heating
source irrespective of the method of heating. This is unlike some of
the work reported in the literature, showing that drying occurs from
the top surface always. Heat transfer through the dried crust was
found to control the drying process in both plate and radiation heating
methods, which was supported by the presence of a constant interface
temperature. In the plate heating the plate contact resistance has also
important effect on the rate of drying. It was possible to predict the
temperature distribution in both methods of heating reasonably well
Heat and Mass Transfer in Freeze Drying 261

Figure 10. Predicted temperature distrbution in freeze-drying of milk, using 2 W

plate heating.

by solving the unsteady state heat conduction equation using finite

differences.

NOMENCLATURE

Cps Specific heat capacity of frozen milk (J/kg K)

Cpe Effective heat capacity of the milk, which includes latent
heat of sublimation of ice (J/kg K)
hc Contact heat transfer coefficient (W/m2 K)
hr Radiate heat transfer coefficient (W/m2 K)
kcr Crust thermal conductivity (W/m k
)
kice Thermal conductivity of the ice (W/m k
)
km Mass transfer coefficient from the surface of the material to
the condense (kg/s m2 bar)
L Height of the substance (m)
Psub Water vapour pressure at the sublimation temperature
(N/m2, or bar)
Pc Water vapour pressure at the condenser temperature
(N/m2, or bar)
q Heat flux (W/m2)
t Time (s)
Tm1 Initial melting temperature (
C)
Tm2 Final melting temperature (
C)
262 Jafar and Farid

Tp Plate temperature (
C)
Tr Radiation temperature (
C)
Ts Surface temperature (
C)
Tsub Sublimation temperature (
C)
w Moisture content (kg water/kg total)
Y Crust thickness (m)
 Thermal diffusivity (m2/s)
" Moisture content (kg water/kg material)
cr Constant related to the permeability of the dried layer
(kg/s m bar)
 Latent of sublimation of ice (J/Kg K)
 Density (kg/m3)

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