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Drying Technology: An International Journal
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Atmospheric Freeze DryingA Review
I. C. Claussen
a
, T. S. Ustad
a
, I. Strmmen
a
& P. M. Walde
b
a
Department of Engineering Science and Technology, Norwegian University of Science and
Technology, Trondheim, Norway
b
SINTEF Energy Research, Kolbjrn Hejes vei 1D, Trondheim, Norway
Version of record first published: 16 Jun 2010.
To cite this article: I. C. Claussen, T. S. Ustad, I. Strmmen & P. M. Walde (2007): Atmospheric Freeze DryingA Review,
Drying Technology: An International Journal, 25:6, 947-957
To link to this article: http://dx.doi.org/10.1080/07373930701394845
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Atmospheric Freeze DryingA Review
I. C. Claussen,
1
T. S. Ustad,
1
I. Strmmen,
1
and P. M. Walde
2
1
Norwegian University of Science and Technology, Department of Engineering Science
and Technology, Trondheim, Norway
2
SINTEF Energy Research, Kolbjrn Hejes vei 1D, Trondheim, Norway
This review article focuses on the development of atmospheric
freeze drying (AFD): technological aspects, product possibilities,
physical properties of products, drying kinetics, modeling, and simu-
lation. The main motivation for developing atmospheric freeze dry-
ing as a new drying technology is the desire to reduce the energy
consumption compared to vacuum freeze drying while maintaining
a high product quality. One technical solution of atmospheric freeze
drying is a combined atmospheric freeze drying and heat pump sys-
tem with new environmentally friendly refrigerants. Temperature
programs make it possible to customize products with desired qua-
lities and properties, like retained color, instant properties, aroma,
and nutritional value.
Keywords Atmospheric freeze drying; Modeling; Physiochem-
ical properties; Review; Technologies
INTRODUCTION
Drying technology has been developing from a tech-
nology mainly used in preservation of foods with the pur-
pose of extension of shelf life as a technology used in
product development, satisfying convenience and quality
demands.
The vacuum freeze-drying process is a well-known and
established technology and a lot has been done regarding
research and development. Energy consumption, product
quality and thermal- and physical parameters during the
drying process are some areas.
[1]
The vacuum freeze-drying
process is used as a benchmark regarding product quality.
Vacuum freeze drying has the advantage of very highly
valued dried products, with nutritional characteristics well
preserved. This was confirmed by Marques et al.,
[2]
who
investigated the physical properties of vacuum freeze dry-
ing of tropical fruits. As expected, vacuum freeze-dried
foods have high values of porosity and low values of
apparent density and conserved color, flavor, and taste.
The main disadvantage is, however, the high fixed and
operational costs. Vacuum operations are mainly batch-
wise, which represents another additional cost, together
with the demanding requirements of apparatus operated
under vacuum.
[3]
An important part of operational costs
is the energy cost, which is high in vacuum freeze drying.
Typical specific moisture extraction rate (SMER) values
for atmospheric freeze drying with heat pumps are in the
range of 4.61.5 kg of water per kWh.
[4]
Likewise, the
SMER of industrial vacuum freeze drying is in the range
of 0.4 or below.
[5]
In order to reduce manufacturing costs,
atmospheric freeze drying was developed.
From a historical point of view, Dr Harold Meryman is
considered the inventor of the science of atmospheric freeze
drying. He showed experimentally that the diffusion of
water vapor from the drying boundary through the dried
shell is facilitated primarily by the vapor pressure gradient
rather than by the absolute pressure in the system. Hence,
it is possible to freeze dry at atmospheric pressure.
[6]
This
proposal resulted in further investigation of the economical
aspects of atmospheric freeze drying.
[7]
A decade later,
Heldman and Hohner
[8]
made an analysis of the process
and derived a mathematical model of simultaneous heat
and mass transfer, describing the moisture content history
of a sample during atmospheric freeze drying. Equations
(1) and (2) represent the heat and mass transfer equations,
respectively, given by Heldman and Hohner:
[8]
qc
p
Mc
p;w

@T
@h

@
@g
k
D
fg
@T
@g
_ _

D
e
D
fg
c
p;w
@P
0
@g
@T
@g
qDH
v
@M
@g
1
eM
w
RT

q
P
0
sat
dM
du
_ _
@P
0
@h

@
@g
D
e
D
fg
@P
0
@g
_ _
2
During the last 15 years, a lot has been done regarding
product development of atmospheric freeze drying. The
Dewatering Laboratory at NTNU and SINTEF in Trond-
heim, Norway, has dried products such as different fish
products,
[9,10]
strawberries and potato,
[11]
starter feed for
the fish industry,
[12]
lactic acid bacteria,
[13]
and sulphite
Correspondence: I.C. Claussen, Norwegian University of Science
and Technology, Department of Engineering Science and Tech-
nology, Kolbjrn Hejes vei 1D, 7491 Trondheim, Norway; E-mail:
ingrid.c.claussen@sintef.no
Drying Technology, 25: 957967, 2007
Copyright # 2007 Taylor & Francis Group, LLC
ISSN: 0737-3937 print/1532-2300 online
DOI: 10.1080/07373930701394845
957
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(wood) pulp.
[14]
The focus in these experiments has been
quality aspects at different drying conditions. The same
research community has also done a lot of work on energy
considerations
[4,15]
and on development of combined
atmospheric freeze drying and heat pump systems using
environmentally friendly working fluids. Research com-
munities in the United States
[16]
and Switzerland
[17,18]
have
done research and development within AFD spray freeze
drying of different pharmaceuticals.
Continuous production line is a key factor in develop-
ing industrial production of atmospheric freeze-dried vege-
tables. The worlds first industrial plant for production
of atmospheric freeze-dried vegetables, Aroma Dry, is loca-
lized in eastern Hungary. In cooperation with the
Norwegian companies Dtech AS and Arctic Aroma,
Aroma Dry develops and produces high-quality atmos-
pheric freeze-dried vegetables for the world market. The
plant started operation in July 2005.
This work is a review of the use of atmospheric freeze-
drying technology, including the technology aspect, pro-
duct variety, measurements of product qualities and
measurements, and modeling and simulation of the physi-
cal properties and drying process. The advantages and
disadvantages of atmospheric freeze drying are discussed,
partly in comparison with vacuum freeze drying.
A selection of articles and books from the first publica-
tions of atmospheric freeze drying back in the 1950s
throght the present have been studied. The range of publi-
cations is, however, limited. From a modeling point of
view, this article concentrates on works either explicitly
on atmospheric freeze drying or works where chamber
pressures of about one atmosphere have been applied.
TECHNOLOGICAL ASPECTS
Overview
The most important atmospheric freeze drying is convec-
tive drying at temperatures below the freezing point of the
product. Compared to vacuum freeze drying, the temperature
is higher, typically in the range of 3 to 10

C. This is due
to the physical properties of humid air, as lower air tempera-
ture reduces the ability to remove moisture. Furthermore,
lower air temperature also requires more energy and therefore
reduces the SMER, expressed as kg moisture extracted per
kWh energy supplied.
[15]
Drying at temperatures around
10

C has proven to be a viable trade-off between quality


and costs, although a faster process is desired.
Rogers et al.
[16]
compared spray freezing into liquid
(SFL) with AFD of a pharmaceutical with vacuum
freeze-dried powder. Compared to vacuum freeze drying,
AFD gave (1) improved heat and mass transfer between
circulating drying medium and the frozen sample, (2)
high quality and homogeneous quality properties of the
dry product with an increased retention of volatile
aromatic compounds in foods, and (3) instead of cake, a fine,
free-flowing powder with a large inner surface area, and
good instant (e.g., wetting and solubility) properties were
obtained. Conclusions were that use of AFD is preferable,
because it enables commercialization of SFL particle engin-
eering technology in the pharmaceutical industry.
[16]
The
advantages of the atmospheric freeze-drying process, in
comparison with vacuum freeze drying, is given in the work
of Li
[19]
as follows: (1) low initial investment cost since
expensive vacuum auxiliary equipment could be elimi-
nated, (2) the process could be designed as a continuous
system with higher productivity and lower operating cost,
(3) the application of a heat pump system and different
process temperature elevating modes in AFD would
decrease energy consumption and drying time, and (4) inert
gas drying environment such as nitrogen or helium can be
applied to minimize the product degradation caused by
oxidation. The main conclusion from his work is that vac-
uum freeze drying still offers the best product quality,
although AFD products show similar characteristics of
rehydration kinetics and hygroscopicity. Only 15%
deterioration of the antioxidant properties was measured
compared to vacuum freeze drying.
[19]
With a few exceptions, most of the literature deals with
atmospheric freeze drying in fluid-bed dryers
[20,21]
and
spray freeze dryers.
[1618,22]
Newer investigations of atmos-
pheric freeze drying in a fluid bed have looked into a pro-
cess where a heat pump system is included with the drying
system.
[15,23,24]
Fluid-Bed Freeze Drying
Conventional fluid beds can be used for atmospheric
freeze drying. The heat and mass transfer is very good in
a fluid-bed dryer where the drying agent passes each unit
of the product. As a consequence, most of the experimental
work done within atmospheric freeze drying has been done
in fluid-bed dryers.
Liquid foods can be frozen and granulated before drying
using a traditional granulator. Another way of making a new
high-quality instant powder is to first put the product under
high pressure together with liquid CO
2
at 30 to 40

C
and then expand it to the surrounding temperature and
pressure. This leads to a considerable foaming of the pro-
duct. The foamed matrix is frozen, granulated, and dried
at freezing temperatures.
[25]
The dried product has very low
bulk density and good instant properties due to its high
porosity. Pieces of foods or small food particles (e.g., peas
and corn) are directly frozen and dried in fluid beds.
Tunnel Freeze Drying
To avoid size reduction caused by mechanical cracking,
tunnel drying is a suitable alternative to fluid-bed drying.
The heat and mass transfer, however, is not as good as in
fluid bed drying. Nevertheless, many experiments on
958 CLAUSSEN ET AL.
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AFD of food products in a tunnel dryer with a heat pump
system have been carried out at NTNU lately. The results
from these experiments are very promising, both regarding
product quality and energy consumption.
[9,26,34]
Fish has been the main food product for product devel-
opment in tunnel dryers in Norway, but other products like
apple and turnip cabbage have also been dried.
[34]
Tunnel
dryers for fish are in general adiabatic, which means that
evaporation heat is supplied by cooling down the drying
air. As drying proceeds, the surface temperature increases
until equilibrium with the air temperature is reached, and
the heat supplied to the drying zone is gradually reduced.
A process speed-up may be obtained by increasing tem-
perature stepwise and thus increase the energy supplied
to the drying zone.
[27]
When foaming of liquid products is not required, a tray
may be used to dry liquids in the tunnel. Non-food
products have also been dried in an atmospheric tunnel
freeze dryer. Rat liver has been dried in an attempt to pre-
serve DNA and RNA for use in biobanks.
[26]
No negative
effects caused by atmospheric freeze drying were found
on the RNA.
Spray Freeze Drying
Within the pharmaceutical industry, spray freeze drying
seems to be a good alternative for producing free-flowing
powder, with high surface area, porous end product, and
good instant characteristics. Enhanced solubility and a uni-
form, ultrafine particle size are the main advantages of this
technology. The methods reported may be classified as (1)
spray freeze drying into liquids (SFL), (2) spray freeze dry-
ing into gases (SFG), and (3) spray freeze drying into gases
over a fluidized bed (SFG-FB).
Spray freeze drying into liquid (SFL) is a new tech-
nology designed to produce nanostructure particles with
high surface area, and AFD is a method for isolating the
particles. Some advantages of SFL-AFDprepared drugs
are high product yields, cryogenic temperature (which pro-
motes drug stability), and that the drugs are molecularly
dispersed in drug=excipient matrices.
[28]
Rogers et al.
[16]
investigated the process as an industrial process for pro-
ducing micronized SFL powders with aqueous dissolution.
The SFL-powders were compared with vacuum freeze-
dried SFL-powders.
Leuenberger
[17]
compared process technologies used for
the size reduction of drug particles. Such technologies were
pyrolysis, milling, classical crystallization, and the use of
supercritical gases, the Glatt vacuum fluid bed system,
spray agglomeration, and spray freeze drying at atmos-
pheric pressure. The spray freeze drying in the cited work
was a spray into a refrigerated air stream (at 60

C),
referred to as spray freeze drying into gases. The author
concludes that the spray freeze drying is the gentlest
process of preparing an instant water-soluble product of
a temperature-sensitive drug. Atmospheric freeze drying
appears to be interesting for a variety of applications.
[17]
In a later work, Leuenberger et al.
[17]
examined the tech-
nical properties of a spray freeze-drying system, denoted
spray freeze drying into gases over a fluidized bed. The pro-
ject encountered problems due to the electrostatic proper-
ties in the product, and the particles were not dried in a
fluid bed but were entrained in the airstream and subse-
quently dried attracted to the matrix of a filter. Solutions
of solids of concentrations as low as 5% were dried. The
particles were frozen in air at 60

C and then sieved and


transferred to a fluid-bed drying chamber. The drying
was done at 1000, 300, and 150 mbar pressure, and the
low-pressure drying was about one third faster than the
near atmospheric drying. The drying temperature was
always kept lower than the glass transition temperature
of the solid. A solution was sprayed over a fluid bed of
dry ice particles. Due to sublimation, bed material had to
be continuously supplied.
[22]
The objective of all the methods is to compensate for
low solubility of certain drugs by reducing particle size.
The particle size, however, may be small regarding fluidiza-
tion properties, and most of the particles must be recovered
from a subsequent filter matrix.
Heat Pump Technology
There has been a significant growth in the potential mar-
ket for heat pump dryers, aided by the impact of new
designs under development or recently introduced to the
market. In a review paper of Chua et al.
[29]
new develop-
ments in heat pump dryers are presented, together with
the potential of incorporating advanced heat pump cycles
for drying applications.
[29]
The most commonly used dryers in conjunction with
heat pumps are batch shelf dryers, tray dryers, and kilns,
but fluid-bed and rotary dryers are also used. Dryers that
consume large amounts of air, for example, flash or spray
dryers, are not particularly well suited for heat pump
operations, according to Chua et al.
[29]
The review gives a
classification scheme for heat pump dryers based on pro-
cessing mode, number of drying stages, number of stages
with heat pumps, types of auxiliary heat input, and heat
pump dryer conditions.
A heat pump dryer is basically a convective dryer, where
heat is transferred by the convection of air. It is more suit-
able for drying solid products than liquid or semi-solid pro-
ducts. Thus, its application at this stage is limited mainly to
solid products.
[30]
Because the construction of continuous
drying systems may require high engineering, modeling,
and design costs, the benefits need to be evaluated on the
basis of cost rather than on energy efficiency alone.
The main advantages of using heat pump technology
are the energy-saving potential and the ability to control
drying temperature and air humidity. This creates the
ATMOSPHERIC FREEZE DRYINGA REVIEW 959
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possibility of a wide range of drying conditions. The
increased demand for ready-to-eat products and con-
venient foods requires well-controlled drying condi-
tions to obtain sufficiently high-quality food products.
Alves-Filho
[31]
examined dried fruits and vegetables, look-
ing at physiochemical properties such as moisture content,
matrix fractions, color, water activity, and bulk density. He
concluded that the results are promising with respect to
producing instant fruits and vegetables by heat pump dry-
ing technology.
[31]
In accordance with Strmmen et al.
[15]
and others, the
use of heat pumps in combination with dryers is of great
importance. Energy consumption is reduced due to the
high coefficient of performance of the heat pump, due to
high thermal efficiency of the dryer when properly
designed. Heat pumps used in drying operations will satisfy
important requirements in industrial drying. Such require-
ments are product quality control, low energy consump-
tion, and reduced environmental impact. A diversity of
lines of research and development in heat pump drying
technologies has been established at SINTEF and NTNU.
A sketch of a heat pump dryer is given in Fig. 1. Several
patents have been granted for products and processes in
the field, and several types of heat pump dryers are being
manufactured internationally.
[23]
Perera and Rahman
[30]
have written a review article
about the potential of heat pump dehumidifier dryers for
use in the food industry. In addition to all the above-men-
tioned advantages, the article also mentions that the con-
densate from the evaporator can be recovered and
disposed of in an appropriate manner. Valuable volatiles
from the condensate are also a potential for recovering.
The drying can also be independent of the ambient weather
conditions, and the use of low temperatures is of great
importance.
Temperature Programs
Temperature programs have been introduced to reduce
drying time, especially in the last drying period. Atmos-
pheric freeze drying in the first step of the drying makes
it possible to preserve the product structure with minimal
shrinkage. After removing the loosely bound water, the
temperature is raised to 1030

C to increase the drying of


the more bound water.
There are at least two reasons in favor of an increasing
temperature (step-up) program: (1) to inhibit solute trans-
port within the product and (2) to enhance heat transport
to the drying zone. This is done by increasing the tempera-
ture gradient from the surface to the drying zone without
exceeding critical temperature limits.
In an adiabatic fluid-bed heat pump dryer, the drying
conditions can be regulated with drying temperatures from
about 20 to 110

C and thus high final product quality is


possible due to temperature regulation. Both step-up and
step-down programs are of importance. Step-down pro-
grams are an option when dealing with products that
experience high freezing point depression during drying;
for example, apples.
Strmmen et al.
[4]
compared properties and quality of
atmospheric freeze-dried cod dried at different step-up pro-
grams. They concluded that lower temperature and longer
residence time at freeze-drying conditions give better pro-
duct quality.
[4]
Optimization of the temperature program
was done by Song,
[32]
who adjusted the sinking speed of fish
feed particles in water by changing the retention period at
freezing temperature before raising the drying temperature.
PRODUCT QUALITY AND INSTANT PROPERTIES
The product quality is of high importance, especially in
the pharmaceutical industry where sensitive single- and
FIG. 1. The heat pump drying unit and components.
960 CLAUSSEN ET AL.
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multicellular structures must be preserved during drying.
The tendency in the food industry is a demand for better
quality, with preservation of taste, color, and nutritional
value in the end product. Instant properties are also of high
importance because of the demand for ready-to-eat pro-
ducts. Atmospheric freeze-dried products must therefore
have comparable qualities to vacuum freeze dried products.
Claussen et al.
[33]
investigated the influence of drying
techniques on the physiochemical, quality, and functional
properties of dehydrated potato water effluent. The para-
meters investigated were color, water content, bulk density,
rehydration properties, sorption isotherms, specific enzyme
activity, solubility, and protein denaturation. The results
from this work indicated that AFD is a gentler drying pro-
cess than spray drying and vacuum freeze drying, since
both enthalpy measurements and sorption isotherms indi-
cated less protein denaturation of AFD samples.
[33]
Alves-Filho
[23]
achieved many improvements by using
atmospheric freeze drying and step-up temperature modes
in drying of pharmaceutical and biotechnological products.
Among the improvements achieved are full reconstitution
of the powder, structure with negligible or minimum
shrinkage, attractive color, active enzymes, inhibition of
protein denaturation, and minimum or no lipid oxidation.
Also, when desirable, a high survival rate of bacteria and
microorganisms is attained. Additionally, the final powder
usually contains undisturbed cell structures, and com-
pounds may be kept in their original form.
[23]
Rogers et al.
[16]
also looked at pharmaceutical products.
They found that atmospheric freeze-dried powders of
danazol had lower surface areas than powders produced
by vacuum freeze drying but significantly greater surface
areas than micronized bulk drug and co-ground physical
mixture. They found similar dissolution profiles for the
atmospheric freeze-dried micronized powder as for vacuum
freeze-dried powder.
[16]
Glycoprotein has also been atmospheric freeze dried and
no structural changes or denaturation, and therefore no
loss of antiviral bioactivity occured during the drying pro-
cess, according to Mumenthaler and Leuenberger.
[18]
The
dried products were mostly obtained in the form of dry,
very fine, and voluminous but still free-flowing powder.
The color and consistency was uniform, and the powder
also had good instant (wetting and solubility) properties.
[18]
In the past few years a lot of work has been done at
NTNU on quality properties of different food products;
for instance, apples, potatoes, fish products, carrots, peas,
and leeks. Indergard et al.
[24]
dried potato cubes in a fluid
bed and investigated properties and quality aspects of the
heat pumpdried instant potato. The instant potato was
studied and compared to vacuum freeze-dried and com-
mercial instant potato products. The results showed that
the new instant potato powder had a higher rehydration
index than both the vacuum freeze-dried and commercially
dried products. The instant powder had a higher bulk den-
sity than vacuum freeze-dried powder but significant lower
bulk density than commercially dried instant potato. The
measurement of color on the different powders was slightly
whiter than commercially produced instant powder, but the
commercially dried powder had a more yellow color than
the other products.
[24]
Atmospheric freeze-dried products seem to have a
superior quality compared to vacuum freeze-dried products,
and this will be of major advantage for this technology with
respect to industrial development. The consumer is today
concerned about quality and is willing to pay for it.
PHYSICAL PROPERTIES AND DRYING KINETICS
The drying kinetics of atmospheric freeze-dried products
depends on (1) drying temperature, (2) material thickness,
(3) operating pressure, and (4) dry matter content. Since
the first innovations to atmospheric freeze drying carried
out in 1959, several scientists have investigated the physical
properties and the drying kinetics in connection with
atmospheric freeze drying of products.
Claussen et al.
[34]
investigated the drying kinetics, sorp-
tion properties, shrinkage, and freezing point depression
during AFD of pieces of apple, turnip cabbage, and cod.
Conclusions from this work were (1) drying temperature
affects the product structure, (2) the product structure
affects the sorption characteristics, and (3) the sorption
characteristics (water activity) affects the freezing point
of the product due to Schwartzbergs equation.
The sample under AFD can be presented schematically
in one dimension as shown in Fig. 2.
Assuming a uniformly retreating ice front and using
sorption isotherms for the solid adsorbent, the following
FIG. 2. Schematic diagram of atmospheric freeze drying.
ATMOSPHERIC FREEZE DRYINGA REVIEW 961
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model for atmospheric freeze drying in a fluid bed of par-
ticulate adsorbent is given in Eqs. (3) and (4) by Wolff and
Gibert:
[35]
AP
0
sat
P
0
c

R
e
R
i
x

m
a
1
a
w
da
w
dY
a
B
r
log
a
w;a
a
w
_ _
_
_
_
_

1
P
0
c
dP
0
c
dt

A
r
expB
r
Y
a

DH
v
M
w
R
T
2
_ _
dT
dt
_ _
0
3
Here, R
e
and R
i
are the external and internal resistances
to combined heat and mass transfer, respectively, defined
as:
R
e

1
b
ext

1
a
ext
DH
s

2
P
0
sat
M
w
RT
2
;
R
i

RT
M
w
D

1
k
s
DH
s

2
P
0
sat
M
w
RT
2
4
More models are given in the following sections, where
modeling and simulations are considered for product units
and the drying system.
Drying Temperature
The effect of air temperature on the rate of AFD of 1 cm
cubes of cooked beef was investigated by Heldman and
Hohner.
[8]
Air temperature was investigated at 3, 8,
and 13

C. The results indicated a greater change in the


predicted drying time than the changes investigated in
any other variable. The practical applications of AFD thus
have to be carefully designed to operate as near the
maximum allowable temperature as possible. Because of
freezing point depression, the drying process has to be
designed individually for each product.
The large dependence of drying rate on air temperature
was found to be caused by two factors. First, higher air tem-
perature resulted in a higher ice core temperature, which in
turn caused a higher saturated vapor pressure at the ice
vapor interface. The higher vapor pressure at the interface
represented an increase in the mass transfer potential and
caused more rapid vapor transport across the porous zone.
The second and minor cause was an increase in the vapor
diffusivity due to increase in temperature.
[8]
Mumenthaler and Leuenberger
[18]
used an aqueous
mannitol solution to find the drying kinetics. The samples
were dried in a fluid bed dryer at 20

C, and the moisture


loss of the samples as a function of time was found. Higher
air flow values mean that the sublimation rate of the sam-
ple could be markedly enhanced, and the total freeze dry-
ing time could be considerably shortened by increasing
the temperature of the circulating medium in the final stage
of the process. It could even be increased above the respect-
ive eutectic temperature of the frozen samples without
affecting the characteristics of the freeze-dried product.
The influence of drying temperature on the drying rate is
acknowledged by several authors that conclude a higher
drying rate at higher temperatures, as expected.
Particle Size
The rate controlling parameter is molecular diffusion of
water vapor within the dry product structure. Heldman
and Hohner
[8]
predicted the effect of sample size on atmos-
pheric freeze drying rate in cubes of precooked beef, and
the results showed a rapid decrease in drying time with
reduced dimension. They stated that for freeze drying with
a very large surface mass transfer coefficient, the time to
dry to any given dimensionless moisture content should
vary with the ratio of the square of the sample size.
[8]
Boeh-Oceancey
[36]
dried pieces of carrot in a fluid-bed
dryer at 5 and 10

C and concluded that drying time


increased as sample thickness was increased. Samples of
limited thickness or below a certain critical value tend to
have higher drying rates in an atmospheric dryer than those
of the vacuum equipment. However, no sample thickness
limit was mentioned.
[36]
Operating Pressure
A minor effect of reducing system pressure on the rate of
freeze drying was found in 1-cm cubes of precooked beef.
Nevertheless, process design for AFD should take full
advantage of the increased drying rate due to reduced sys-
tem pressure in the drying chamber.
In 1959, Meryman
[6]
already had a theory that indicated
that the vapor pressure gradient, rather than the absolute
pressure of the system, is the main source for the passage
of water vapor from the drying interface through the dried
part of a product. He also confirmed this through experi-
mental work. His conclusions regarding the factors deter-
mining the rate of diffusion of water vapor through the
dried part of a product are (1) rate of vapor production
(specimen temperature), (2) resistance of the dried layer,
and (3) water vapor pressure at the product surface.
Dry Matter Content
Coffee extract solutions were investigated by
Boeh-Ocansey
[37]
to see the effect of increasing the product
concentration on drying rate. Increased concentration pre-
drying resulted in a reduction of vapor pressure difference
between the ice front and the surface of the product, lead-
ing to a reduction on the drying rate. The results are given
in Boeh-Ocansey.
[37]
Economic Considerations
Woodward
[7]
did some economic analysis that also
indicated that energy costs for moisture removal can be
equivalent to vacuum freeze drying. The energy cost was
also investigated in 1990 by Wolff and Gibert,
[21]
and the
result was that even though processing time is longer with
962 CLAUSSEN ET AL.
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atmospheric freeze drying than vacuum freeze drying,
energy savings of 35% can be expected from a continu-
ous-duty facility. The dehydration kinetic tests were carried
out on a model biological product (potato slices).
Preliminary evaluation of energy requirements of a
processing cycle was proposed by Donsi et al.
[38]
They
compared vacuum- and atmospheric freeze-dried shrimps
and determined the freeze-drying kinetics in both cases.
Their conclusions were a reduction in the energy costs of
the single-stage freeze-drying process of 30%, provided
that the freeze-drying stage is carried out at atmospheric
pressure.
[38]
Mumenthaler and Leuenberger
[18]
studied the drying
kinetics of some biologically active substances and some
liquid foods. They investigated commercial liquid foods
with different characteristics, like (1) milk products with
a high amount of lipids, and therefore leading to freeze-
dried samples with poor instant properties; (2) orange juice
with very high concentration of carbohydrates (mainly
sucrose), and therefore leading to end products with very
hygroscopic properties; and (3) coffee extract, a real chal-
lenge for the freeze-drying process, due to the very high
quality requirements (color, taste, volatile flavor compo-
nents) claimed for the dehydrated products.
Strmmen et al.
[39]
studied drying of leeks, where differ-
ent conditions and moisture contents were used to study
possible effects on physical properties and quality. The
effective mass diffusivity was determined from drying
kinetics data and was described using a two-dimensional
flat-plate Fickian model. The result shows an increase of
effective mass diffusivity with the drying temperature and
an increase with moisture content and smaller sized
slabs.
[39]
MODELING AND SIMULATION
Modeling and simulation of AFD can be divided into
two categories. The first category is modeling and simula-
tion of product units. The heat and mass transfer inside a
given product is modeled, and the conditions in the drying
chamber are used in the derivation of the internal transport
equations or their boundary conditions. The second cate-
gory is modeling and simulation of the drying system itself.
Here, the emphasis is on the conditions in the drying cham-
ber, and usually only the total heat and mass transfer to
and from each product unit is modeled.
Modeling and Simulation of Product Units
The most common kind of product model is a receding
ice front model. In this type of model, the product is div-
ided into two layers: a frozen (or wet) inner core and a
dry outer layer. It is assumed that drying occurs by the
frozen core gradually shrinking down to zero. This assu-
mption defines a receding interface between the frozen
and dry layersthe ice frontwhere heat transported
from the surface of the product is used for sublimation of
nearby ice. The resulting water vapor is transported back
to the surface and to the ambient atmosphere. This transfer
of heat and vapor through the dry layer is modeled by a
system of transport equations (e.g., Eqs. (1), (2), and (7)
or Eqs. (5) and (6)), and the heat and mass transfer between
the product surface and the atmosphere is often assumed to
be purely convective. When given the initial product tem-
perature and moisture content, as well as appropriate
boundary conditions at the ice front and the product sur-
face, solving the equation system yields the evolution in
time of the temperature and moisture profiles inside the
product unit.
To keep this kind of moving boundary problem math-
ematically simple, authors typically consider regular pro-
duct geometries (such as spherical, cylindrical, cubical, or
slab-type shapes) and one-dimensional heat and mass
transfer along a characteristic dimension, such as the diam-
eter of the product unit. Quasi-steady-state conditions,
allowing one to consider equality between inner and outer
heat and mass transfer, are also commonly assumed. This
kind of receding ice front model, where the whole ice front
moves as one object, is commonly referred to as a uni-
formly retreating ice front (URIF) model.
Sandall et al.
[40]
used a one-dimensional URIF model in
their study of drying of precooked turkey breast meat.
They studied drying at near vacuum chamber pressures,
as well as drying in inert nitrogen and helium atmospheres
of pressures up to 760 mmHg (1 atm). Heat and mass
transfer parameters were also modeled. The drying simula-
tions showed good agreement with experimental results
during removal of the first 7590% of the water, but the
predicted drying rates were too high for the remaining part
of the process.
Hill and Sunderland
[41]
looked at freeze drying of beef
under near vacuum conditions and under atmospheric
pressure. They considered a one-dimensional model where,
in addition to diffusive transport, internal convective trans-
port under different porous medium flow regimes (free
molecule, transition, and continuum flows) were studied.
Wolff and Gibert
[35]
used a one-dimensional URIF
model together with adsorption isotherms to derive a
model for AFD in a fluid bed of adsorbent. The URIF
basis transport equations for this model were
m
0
d1 X

dt

A
DH
s
1
a
ext

s
k
s
_ _
1
T
c
T
front
5
m
0
d1 X

dt
A
1
b
ext

RTs
DM
w
_ _
1
P
0
front
P
0
c
6
By using another equation to couple Eqs. (5) and (6)
and introducing the effect of adsorption, they designed a
model for homogeneous and isotropic products shaped like
ATMOSPHERIC FREEZE DRYINGA REVIEW 963
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1
2

plates, cylinders, or spheres. Simulation results and experi-
mental results were compared for square, 3-mm-thick
flakes of potato in a fluid bed with gelatinized starch par-
ticles of size 150 mm. Good agreement was found.
Several authors have built on Wolff and Giberts work,
among them Lombra~ nna and Villaraan,
[20,42]
who also stud-
ied AFD in a fluid bed of adsorbent. The product units
considered were spherical particles, and a one-dimensional
modified URIF model in the radial direction was pre-
sented. It was assumed that the bed was completely mixed
and that the effective physical parameters were spatially
uniform in each of the two layers. Product shrinkage effects
were represented implicitly by changes in the transport
coefficients, thereby influencing the drying rate. Lombra~ nna
and Villaraan
[20]
studied drying of 2- to 4-mm-wide calcium
alginate particles and 1-mm-wide wetted food paste parti-
cles using starch and Baylith WE G 291 zeolite as
adsorbents. They used experimental data to determine
transport parameters and degree of product shrinkage
and compared the corresponding simulated drying rates
with the observed ones. Lombra~ nna and Villaraan
[42]
studied,
using the same model as above, the influence of chamber
pressure and temperature on this process for 2-mm-wide
cereal food paste and Baylith WE G 291 zeolite adsorbent.
Different drying strategies, with chamber pressures ranging
from 310 to 760 mmHg and temperatures ranging from
10 to 40

C were tested.
Not all authors have limited themselves to one spatial
dimension. Heldman and Hohner
[8]
first derived a dimen-
sionless URIF-type model for one dimension and then
extended it to a kind of three-dimensional model for cubes
where heat and mass transfer were considered separately in
the three spatial dimensions. In one dimension, the trans-
port equations they used are given in Eqs. (1) and (2).
The boundary condition at the icevapor interface was

kL
D
fg
@T
@g

gg
iv
DH
s
D
e
s
D
fg
@P
0
@g

gg
iv
g
iv
q1 M
0
c
p;i
@T
@g
7
The models were used for simulation of drying of
precooked beef. In the one-dimensional case, the results
supported the above-mentioned observations of Sandall
et al.
[40]
In the three-dimensional case, the simulations com-
pared well to experimental results for mean dry basis
moisture content above 0.1.
Li
[19]
presented a film sublimation model that coupled a
fluid dynamics model for the ice-vapor interface with a
URIF model for the vapor transport through the dry,
porous zone. The interface model considered a vapor film
resulting from sublimation from an imagined ice wall under
local thermodynamic equilibrium. The description of the
diffusive vapor transport from the interface was made to
work with flow problem formulations in the Fluent CFD
package. Fluent was used for simulation of drying of a
plate of ice, a chitosan membrane, and a 10-mm-wide cube
of apple at temperatures 4, 8, 12, and 16

C. Com-
parisons with experimental results showed good agreement,
mainly for medium and low moisture contents and the
highest drying temperatures.
Li also compared experimental results for 10-mm apple
cubes under different constant=ascending temperature con-
ditions with a pure Fickian mass diffusion model with con-
stant effective diffusivity, D
e
. He incorporated empirical
Arrhenius expressions for D
e
and a shrinkage parameter
(linear in total moisture content) into Eq. (8) and achieved
good agreement with the experimental results.
Xt X
e
X
c
X
e

8
3
p
6

1
n0
1
2n 1
6
exp 2n 1
2
3p
2
D
e
t
4L
2
_ _
8
Modeling and Simulation of Drying Systems
A few different AFD techniques have been developed
over the last decades, and some authors have made efforts
to model these techniques and simulate them. Many system
models consider different variants of fluid-bed drying, a
technology that offers good heat and mass transfer
between the product and the drying medium.
Kutsakova et al.
[43]
modeled AFD of granulated pro-
ducts in cold air cylinder dryers. They considered a process
where the outer dry layers of the granules were continu-
ously removed, so that modeling the process could be done
by just considering sublimation of frozen granules. The
resulting shrinkage of these frozen granules was modeled
by a system of equations involving the chamber height,
air and particle flow parameters, and the highest air tem-
perature feasible (without the ice melting). The model
was used in a simple case to derive a granule residence time
for a given final granule radius.
Menshutina et al.
[44]
modeled AFD in a spouted bed
using equations of heterogeneous media mechanics for
modeling hydrodynamics and drying kinetics. The energy
efficiency of the process was investigated in drying of fro-
zen spherical particles of mannitol solution, with a mean
particle size of 150 mm and a bed temperature of 20

C.
This AFD process was found to be more energy efficient
than the corresponding vacuum freeze-drying process.
Tomova et al.
[45]
studied a batch fluid-bed AFD process
with spherical particles of c-Al
2
O
3
and cubical pieces of
carrot as products. They modeled the heat and mass trans-
fer between the bed and product units using a one-dimen-
sional heterogeneous two-phase fluid-bed model. They
assumed monodisperse, spherical product particles and
that the heat transfer between the bubbles and the suspen-
sion and walls could be neglected. Comparisons of simula-
tion results for different material loads and different inlet
964 CLAUSSEN ET AL.
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and outlet air temperatures with experimental results
showed good agreement.
Alves-Filho
[46]
studied the use of heat pumps in drying
of fruits and roots. He considered a Fickian diffusion
model for the product and used it to develop a simulator
for heat pumpassisted fluid-bed drying. Several key
aspects of heat pumpassisted combined AFD=above-zero
air-drying schemes were simulated, including bed tempera-
ture and humidity, product moisture content, and energy
efficiency. Simulations were carried out for apples, with
ammonia or R12 as the refrigerant.
A very different kind of consideration is that of
Bruttini,
[47]
who modeled long-term conservation of a
mummy in a conservation cell. Moisture in the air inside
the cell was collected as ice on the cell walls, which were
kept at 6

C. The mummy was modeled quite crudely as


a parallelepiped with uniform transport properties, but
the model itself was comprehensive, three-dimensional,
and transient, including moving ice-air interfaces and con-
ductive, convective, and radiative heat transfer.
[47]
DISCUSSION AND CONCLUSIONS
Atmospheric freeze drying has a relatively long resi-
dence time because of internal resistance to mass transfer.
Minimizing product size and thickness reduces the drying
time considerably, and 2 mm has been a limit for economi-
cal reasons. In combination with heat pump technology,
atmospheric freeze drying seems to be an environmentally
friendly and economically favorable technology compared
to vacuum freeze drying.
Atmospheric freeze drying can be used to dry a variety
of products within several product categories, both solid
and non-solid products (when pretreated before drying).
Compared with vacuum freeze drying, the atmospheric
freeze-drying process will be more complicated when
liquids are dried because of the need for pretreatment,
either spray freezing or foaming.
It seems like atmospheric freeze drying is a favorable
technology, both because the process produces high-quality
products and the fact that vacuum equipment is of high
cost. Fluid-bed dryers can be made simple and, combined
with a heat pump system, they might be competitive in
the food industry and the pharmaceutical industry, where
vacuum freeze dryers are widely used today.
Despite all previous investigations, there is still a need to
obtain data on the physical properties of both foods and
non-foods and to develop suitable drying models. Use of
heat pump technology in combination with the drying
process is also necessary to reduce the energy consumption.
NOMENCLATURE
AFD Atmospheric freeze drying
DNA Deoxyribonucleic acid
NTNU Norwegian University of Science and
Technology
RNA Ribonucleic acid
SFL Spray freeze drying into liquid
SINTEF Foundation for Scientific and Industrial
Research at the Norwegian Institute of
Technology
SMER Specific moisture extraction rate
(kg H
2
O=kWh)
URIF Uniformly retreating ice front
A Exchange surface (m
2
)
A
r
Constant
a
w
Water activity
a
w,a
Water activity of the adsorbent
B
r
Constant
c
p
Specific heat of dry product at constant
pressure (J=[kg K])
c
p,i
Specific heat of ice at constant pressure
(J=[kg K])
c
p,w
Specific heat of liquid water at constant
pressure (J=[kg K])
D Dry layer water vapor diffusivity (m
2
=s)
D
e
Effective water vapor diffusivity (m
2
=s)
D
fg
Water vapor diffusivity for free gas
(air vapor) (m
2
=s)
DH
s
Latent heat of sublimation (J=kg)
DH
v
Latent heat of vaporization (J=kg)
L Sample half-thickness (m)
M Dry basis moisture content
M
0
Initial dry basis moisture content
M
w
Molar mass of water (kg=mol)
m
0
Initial mass of water (kg)
m
a
Mass of water in the adsorbent (kg)
P
0
Partial pressure of water vapor (Pa)
P
0
c
Partial pressure of water vapor in the drying
chamber (Pa)
P
0
front
Partial pressure of water vapor at the
sublimation front (Pa)
P
0
sat
Water vapor saturation pressure (Pa)
R Molar gas constant (J=[K mol])
R
e
External combined heat and mass transfer
resistance ([Ns]=kg)
R
i
Internal combined heat and mass transfer
resistance ([Ns]=kg)
s Dry layer thickness (m)
T Temperature (K)
T
c
Temperature in the drying chamber (K)
T
front
Temperature at the sublimation front (K)
t Time (s)
X (Total) moisture content (kg=kg)
X

Remaining fraction of initial mass of water


in product
X
c
Critical moisture content (kg=kg)
ATMOSPHERIC FREEZE DRYINGA REVIEW 965
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2

X
e
Equilibrium moisture content (kg=kg)
x Distance (m)
Y
a
Absolute humidity of the adsorbent
Greek Symbols
a
ext
External heat transfer coefficient (W=[m
2
K])
b
ext
External mass transfer coefficient (kg=[Ns])
e Porosity
g Dimensionless distance (s=L)
g
iv
Dimensionless position of the icevapor
interface
h Dimensionless time (D
fg
t=L
2
)
k
s
Dry layer thermal conductivity (W=[mK])
q Bulk density of porous zone (kg=m
3
)
u Relative humidity
ACKNOWLEDGEMENT
The Norwegian Research Council is acknowledged for
financing this survey.
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