food and bioproducts processing 8 7 ( 2 0 0 9 ) 8795

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Food and Bioproducts Processing

journal homepage: www.elsevier.com/locate/fbp

Comparing the crystallization of sucrose and lactose

in spray dryers
Md. Imtiaz-Ul-Islam , T.A.G. Langrish
Drying and Process Technology Group, School of Chemical & Biomolecular Engineering, Building J01,
The University of Sydney, Darlington, NSW 2006, Australia

a b s t r a c t
The relative extent of crystallization for lactose and sucrose within spray dryers allows the WLF equation to be tested
for this type of in-process crystallization, since this equation suggests that the crystallization rate is related to the
difference between the material temperature and the glass-transition temperature of that particular material. In this
study, the amount of sucrose crystallization during drying was studied using a bench-top spray dryer (Buchi B290)
over a practical range of inlet gas temperatures (95220 C). It has been found that very large changes in the degree of
crystallinity for the nal spray-dried product can be achieved for sucrose by using different inlet gas temperatures,
compared with much smaller changes in the crystallinity of lactose for a similar range of inlet temperatures. This
result supports the suggestion that the crystallization rate is related to the difference between the material temperature and the glass-transition temperature, since sucrose has a much lower glass-transition temperature than
lactose. The results have the potential to be implemented to achieve specied degrees of crystallinity in many powder
materials produced from spray-drying processes.
2008 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.
Keywords: Stickiness barrier; Sucrose; Crystallization kinetics; WLF equation; Operating condition(s)

1.

Introduction

Spray drying is a potential process to obtain crystalline powders in a single step, rather than multi-stage conventional
crystallization processes where crystallization is normally followed by a further drying step. Lactose and sucrose have the
same molecular weight, but due to the difference in their
molecular conguration they have different glass-transition
temperatures (Slade and Levine, 1994). Spray drying of sucrose
is known to be difcult because its glass-transition temperature is low (62 C; Roos, 1993), making this material sticky
at low drying temperatures (Bhandari et al., 1997b; Bhandari
and Howes, 1999). However, recent work on combining the
drying and crystallization processes (Chiou et al., 2008a,b) suggests that drying at temperatures above the glass-transition
temperature hastens the subsequent transition from a sticky
amorphous material to a less sticky crystalline one. Hence
continuing the transformation from a sticky amorphous material right through to the less sticky crystalline state by
operating the dryer at a sufciently high temperature may

assist in the spray drying of sucrose by creating more crystalline sucrose at these high temperatures.
The WilliamsLandelFerry equation (Williams et al., 1955)
has been applied to many polymer systems to nd the rate
of crystallization as a function of the material temperature
(T) and the glass-transition temperature (Tg ) at constant temperature and controlled humidity conditions (Bhandari and
Howes, 1999; Roos and Karel, 1992, 1991a,b, 1990; Levine and
Slade, 1986; Soesanto and Williams, 1981). Also, both the
glass-transition temperature (Tg ) and the difference between
material and glass-transition temperatures (T Tg ) have been
used to dene and/or evaluate material properties such as
crystallization (Bhandari and Howes, 1999), caking, lumping
and agglomeration (Bhandari and Howes, 1999; Aguilera et
al., 1995), the effect of storage conditions on retaining specic material properties (Paterson et al., 2005; Bhandari and
Howes, 1999; Senoussi et al., 1995; Schenz, 1995), the effects
of conditions for reactions to take place (Meste et al., 2002;
Buera and Karel, 1993), and to measure the diffusion rate constant during curing (Wise et al., 1997). Again, almost all of

Corresponding author. Tel.: +61 2 93515661; fax: +61 2 9351 2854.

E-mail address: i.islam@usyd.edu.au (Md. Imtiaz-Ul-Islam).
Received 4 July 2008; Received in revised form 22 September 2008; Accepted 25 September 2008
0960-3085/$ see front matter 2008 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.
doi:10.1016/j.fbp.2008.09.003

88

food and bioproducts processing 8 7 ( 2 0 0 9 ) 8795

temperature with all other parameters being the same. Since

the particle continuously loses moisture through drying, the
glass-transition temperature (Tg ) also changes and can be predicted by the Gordon and Taylor (1952) equation.
In this paper, we refer to previous work carried out by Chiou
et al. (2008a) on lactose, with inlet gas temperatures in the
dryer between 134 C and 210 C. They found that the degree of
crystallinity for lactose could be altered by about 10% over this
temperature range. For sucrose, it might be expected, on the
basis of sucrose having a lower glass-transition temperature
(62 C) than lactose (101 C; Roos and Karel, 1991b) and the WLF
equation, that the degree of crystallinity might be altered more
signicantly for sucrose than for lactose over the range of inlet
gas temperatures from just below 100 C to 220 C.

Fig. 1 Schematic diagram showing the gas and particle

temperature prole throughout the dryer.
these temperature and moisture-dependent physical and/or
chemical phenomena in polymer and food systems have
been extensively reviewed by justifying the applicability of
the glass-transition concept and the WLF equation in those
systems (Rahman, 2006; Meste et al., 2002; Champion et al.,
2000). However, there have been few studies done regarding
the applicability and implementation of the WLF equation
under dynamic conditions, such as the spray-drying process. It has been suggested (Busin et al., 1995) and found
(Bhandari and Howes, 1999; Bhandari et al., 1997b) that the
glass-transition temperature is the single most important
parameter for assessing the ability of sugars and sugar-rich
materials to be spray dried.
The WLF equation can be applied to conditions that give
both drying and crystallization (Chiou et al., 2008b), where
the rate of crystallization is related to the temperature difference (T Tg ). During spray drying, the material temperature
(T) is the particle temperature and changes throughout the
dryer, as drying occur. The temperatures of the particles tend
to approach those of the gas very quickly after the start of the
dryer (Ozmen and Langrish, 2003), and in cocurrent spray drying, the gas temperature drops very quickly after the start of
the dryer. This situation means that the nal (outlet) solids
temperature, Tp , is often very close to the nal (outlet) gas
temperature (Fig. 1).
The temperature prole of the particles and the gas along
the spray dryer has been explained in Ozmen and Langrish
(2003). Fig. 1 shows schematically that the temperature of the
particles approaches the gas temperature very closely just
after spraying the liquid feed. Fig. 1 also represents schematically the quantitative gas and particle temperature proles
from simulations, as reported in Langrish (2008). The glasstransition temperature (Tg ) and the material temperature can
be used in the WLF equation to predict the solid-phase crystallization rate at any stage of drying. The rate can then be
integrated throughout the particle residence time in the dryer,
even when the gas and particle temperatures and the particle moisture contents are changing. This procedure has been
described in detail by Chiou et al. (2008b).
The WLF equation shows that the rate of crystallization
can be increased by increasing the value of the temperature
difference (T Tg ). By increasing the inlet gas temperature,
while maintaining the other variables constant, the material temperatures throughout the dryer can be increased,
because outlet temperature is directly related to the inlet

2.

Methods and materials

2.1.

Materials

In these experiments, pure sucrose monohydrate (C12 H22 O11 )

(analytical-grade reagent from Ajax Finechem Pty Ltd., Australia for purity) has been used as the test material.

2.2.

Sample preparation

Sucrose solutions of 20% (w/w) concentration were prepared

by adding sucrose in tap water over a temperature range from
25 C to 30 C. A magnetic stirrer was used to enhance the
dissolution rate of the sucrose so that a clear solution was
obtained without any visible crystals being present.

2.3.

Spray-drying operating conditions

The solutions were spray dried using a Buchi-B290 Mini Spray

Dryer with inlet temperatures ranging from 45 C to 220 C,
an aspirator setting of 100% (38 m3 /h), pump settings of 3, 5,
and 10% (1.1, 1.5, and 3 ml/min respectively), and a nozzle air
ow rate of 601 l/h (50 on the nozzle rotameter scale). These
operating conditions caused the outlet temperature to be in
the range of 36 C to 142 C.

2.4.
Moisture sorption and moisture content
measurement
Crystallization behaviour was studied according to the
method described in previous work (Imtiaz-Ul-Islam and
Langrish, in press). However, for these set of experiments,
a mass of 0.55 g of the powder product obtained just after
spray drying the sample solution was placed on a Petri dish
as a monolayer (one particle thick), and the mass change as a
function of storage time was recorded (by computer using the
Mettler Toledo Balance Link v3.01 program) once per minute
over a period of 12 days until the mass of the sample and dish
stayed constant for more than 6 h. Afterwards, a moisture content measurement was done by oven drying the samples for
24 3 h at 100 C.

2.5.

Analytical experiments

Both the original (raw) sample, and the product dried at a high
inlet gas temperature (220 C) and the lowest pump rate (3%),
were assessed and compared, in order to investigate possible
thermal degradation of the spray-dried products using the following analytical techniques and procedures. These analytical

food and bioproducts processing 8 7 ( 2 0 0 9 ) 8795

89

tests were performed to assess any thermal degradation of

the spray-dried powders, because at these drying conditions
sucrose might break down into smaller sugar units, and these
units might polymerize to form other polymers.

rent between 40 and 80 A. The images were captured using

the software ImageSlave v2.11.

3.

Results and discussion

2.5.1. Modulated differential scanning calorimetry

(MDSC)

3.1.

The stickiness barriera hypothesis

The glass-transition temperatures of the powders were

determined by modulated differential scanning calorimetry
(MDSC). Samples for MDSC measurements were prepared
accordingly to standard procedures using hermetically sealed
pans. The samples were heated from 35 C to 200 C using
a ramp rate of 5 C/min with a 1 C modulated signal every
60 s using a modulated differential scanning calorimeter (TA
Instruments Q1000).

At lower inlet gas temperatures (below 100 C), the yield of

sucrose has been found to be signicant (Table 1). The yields
go through a peak as the inlet gas temperature is increased,
before approaching zero at higher inlet gas temperatures. This
trend in yield has also been observed by other researchers
(Bhandari et al., 1997a). At lower gas temperatures, it is
expected that the moisture contents of the particles are signicant compared with those at higher gas temperatures, and the
glass-transition temperatures of the outlet solids are therefore
lower than at higher temperatures. This situation means that,
as the gas temperatures increase, the glass-transition temperatures also increase as the outlet moisture contents decrease,
making the particles less sticky up to the point where the
increase in gas temperature no longer changes the outlet
solids moisture content signicantly. This process explains
why the yields increase initially. In spray drying, the moisture content of the wet and heavy product that is produced
at these lower inlet air temperatures also depends on the liquid feed concentration, the liquid feed rate and its dispersion
(droplet size), the inlet gas velocity and the particle residence
time.
The yields then decrease as the gas temperature increases
above about 6585 C, when the outlet moisture contents and
hence the glass-transition temperatures do not change significantly with changing gas temperature, but the increasing gas
temperatures means that the particle (material) temperatures
increase signicantly, making the amorphous particles that
are initially produced more likely to be sticky. This process,
which is well known, explains the peak in yield and the low
yields at temperatures immediately above this peak in yield.
This zone of low yields could be described as a Stickiness
Disaster.
The new nding here is that there is a region, above the
zone of low yield, The Stickiness Barrier (Fig. 2), where the
yields increase signicantly again. The explanation, as will be
demonstrated, is that the temperature difference (Tp Tg ) in
this high-temperature region is sufciently high for crystallization to occur, as suggested by Chiou et al. (2008a). This
crystalline product is likely to be much less sticky than the
amorphous products produced at lower inlet gas temperatures, increasing the yields as shown in Table 1 and Fig. 2.
Chiou et al. (2008a) showed that, for lactose, the degree of crystallinity could be changed by about 10% for changes in the inlet
gas temperatures from 134 C to 210 C. For sucrose, the lower
glass-transition temperature of 62 C than lactose (101 C) suggests, when considering the temperature difference (Tp Tg )
which is the driving force for solids-phase crystallization, that
more crystallization could occur for sucrose (over the inlet gas
temperature ranges used here, from 45 C to 220 C) than for
lactose. These ndings appear to conrm this expectation. The
stickiness barrier concept is the idea that stickiness appears
to stop the use of higher drying temperatures. However, we
show here that higher drying temperatures, if sufciently
high, can be used to crystallize the materials, making them
less sticky and improving the yields. It is demonstrated here
that this barrier can be overcome with sufciently high drying
temperatures that crystallize the material. We suggest that

2.5.2. Liquid ChromatographyMass Spectrometer

(LCMS)
For assessing the possible thermal degradation of the sucrose,
Shimadzu Prominence Ultrafast Liquid Chromatograph (UFLC)
coupled to a mass spectrometer consisting of the following
modules was used in this study: vacuum degasser (DGU20A5), high pressure mixing pumps (LC-20AD), autosampler
(SIL-20A), column oven (CTO-20A), single quadrupole mass
spectrometer (LCMS-2010EV), and system controller (CBM20A). The parameters used for LCMS analysis were 0.2 ml/min
ow rate, 10 l injection volume, ESI interface, 5 kV cone voltage, 1.5 kV detector voltage, 1.2 ml/min nebulizer ow, and
50-2000 m/z mass scan range. The samples were prepared
by dissolving them in 10 mM CH3 COONH4 and then diluting them with CH3 CN to a nal concentration of 70% CH3 CN
and 0.5 mg/ml sucrose. The solutions were centrifuged at
3500 min1 for 10 min, and the supernatant was transferred
into autosampler vials.

2.5.3.

Fourier Transform InfraRed (FTIR)

To conrm the absence of thermal degradation for the sucrose,

a Varian Schimitar 2000 equipped with a PIKE ATR accessory
and Resolutions Pro v4.1.01 software was also used in this
study. The parameters for FTIR analysis were: sensitivity 1,
5 kHz speed, 1 UDR, 1:4 resolution cm, 32 total scans. For FTIR
analysis, the samples were used as supplied and compressed
on the ATR surface using a pressure of 17 and 19 psi for raw
and spray-dried sucrose, respectively.

2.5.4.

Ion Chromatography (IC)

A third test for thermal degradation was the use of a Dionex

ICS-3000 Ion Chromatography System. The system was congured, operated and controlled by software called Chromeleon
(version 6.70) from a server PC. The following module and settings were used for sugar analysis, CarboPac PA1, PA1 guard
column, 16 mM sodium hydroxide eluent, 0.1 ml/min ow rate,
50 l injection volume, and pulsed amperometry, gold electrodes for sample detection.

2.6.

Scanning electron microscope (SEM)

Samples of the powders were prepared by placing a small

amount of the samples onto a carbon tape on an aluminium sample stab. The sample was given a standard 45 nm
gold/platinum coating to produce the conductive surface. The
electron micrographs were produced using a Philips SEM 505
scanning electron microscope (SEM) in secondary electron
mode with operating conditions of 10 keV and a lament cur-

90

44 (1)
23 8 (4)
3 0.4 (2)
32 (1)
20 5 (2)
<1 0.1 (3)
24 3 (2)
9 4 (3)
<1 0.4 (3)
1 (1)
<1 (2)
<1 0.05 (3)
<1 (1)
<1 (1)
<1 0.2 (3)
<1 (1)
<1 (1)
<1 0.3 (3)

Fig. 2 The concept of a stickiness barrier for spray drying

sucrose and other sugar-rich materials.

Fig. 3 Yield of the spray-dried products at different inlet

gas temperatures.
the stickiness barrier is related to the difference between
the material temperatures and the glass-transition temperatures of the materials. We argue that a similar stickiness
barrier should exist for the spray drying of other carbohydrate polymers and that a knowledge of their glass-transition
temperatures can be used to guide the selection of operating conditions to overcome the barrier, by selecting inlet
temperatures that are sufciently above the glass-transition
temperatures to crystallize the materials without thermally
degrading them.
The stickiness barrier has been observed irrespective of
different pump rate (feed rate) within the same temperature
range (Figs. 3 and 4). However, the product yield was higher
at lower liquid ow rates, for a number of possible reasons.
One reason is that the particles may have crystallized faster
at lower liquid ow rates than at higher ones due to being
heated more quickly to higher temperatures, from a heat balance between the gas and the particles. Another reason is that
the droplet velocities from the nozzle are higher at higher

Yield, % (mean standard

deviation, number of runs)

3%
5%
10%

4 (1)

14 1(2)
<1 (2)
3 (1)

4 (1)
8 4 (3)
10 (1)

8 (1)
7 7 (3)
9 9 (3)

120
105
85
65
45

Pump rate

Table 1 Average yields of the spray-dried products at different inlet gas temperatures.

95

Inlet gas temperature ( C)

160

200

210

220

food and bioproducts processing 8 7 ( 2 0 0 9 ) 8795

Fig. 4 Yield of the spray-dried products at different outlet

gas temperatures.

91

<1 (1)
<1 0.3 (4)
<1 0.1 (2)
<1 (1)
<1 0.2 (2)
9 4 (3)
<1 0.01 (2)
<1 0.3 (3)
11 1 (3)
8 (1)
9 1 (2)
10 2 (3)
20 3 (2)
15 (1)
15 3 (3)
16 (1)
17 (1)
18 9 (3)
9 (1)
13 4 (3)
9 2 (3)
8 (1)
6 2 (3)
10 (1)
4 4 (2)
9 9 (2)
1 (1)
13 (1)

3%
5%
10%
Peak height (mean standard
deviation, number of runs)

200
160
120
105
95
85

It has been established (Imtiaz-Ul-Islam and Langrish, in

press; Lehto et al., 2006; Buckton and Darcy, 1996) that the
peak heights (change in moisture content, % (100 kg kg1
dry basis)) from moisture sorption experiments represent the
extent of crystallinity of the samples, as demonstrated by
comparisons between moisture sorption tests, X-ray diffraction tests and differential scanning calorimetry, provided that
the particle layers in sorption tests are kept sufciently thin,
as here (less than 1 mm). Thus, the peak heights obtained for
the samples in this study give the overall picture of crystalline
behaviour for sucrose obtained at different operating conditions over a range of inlet gas temperatures from below 100 C
to 220 C and a range of liquid ow rates into the dryer, which
affect the material temperatures within the dryer and the outlet temperatures for the particles and the gas from the dryer.
The products that were spray-dried at both low temperatures (below 100 C) and high temperatures (above 200 C)
were found to be more crystalline in nature, according to their
low sorption peak heights, than those produced at intermediate temperature conditions. However, at very low inlet gas
temperatures, the particles had high moisture contents and
showed amorphous characteristics, producing relatively large
peak heights (Fig. 5) and giving low yields (Fig. 3).
The two major operating parameters in this study, inlet
gas temperature and the pump (liquid ow) rate, have interacting effects on both the yield and the crystallinity of the
particles. It would be expected that higher inlet gas temperatures and higher liquid ow rates would give similar particle
temperatures (and similar outlet gas temperatures) to those

65

Moisture sorption characteristics

45

3.2.

Inlet gas temperature ( C)

liquid ow rates, so the amount of direct inertial deposition

of droplets and particles on the walls is higher than at lower
liquid ow rates (Hanus and Langrish, 2007).
The characteristic behaviour, for higher inlet gas temperatures above 200 C, was that the product came off the dryer
and cyclone walls as the dryer cooled down, suggesting that
crystallization has occurred on the walls of this small-scale
equipment and not during particle drying in the gas. Despite
this apparent crystallization process on the walls of the equipment, the collected powder was very free-owing and was not
agglomerated signicantly, indicating that the crystallization
process on the walls has not caused caking of the powder products. Considering the potential for scale up of this process,
commercial spray dryers have larger residence times (60 s or
more) compared with this equipment (about 1 s), so there is
some potential for carrying out the crystallization process for
sucrose in commercial spray dryers without relying on collecting sucrose from the dryer walls.

Pump rate

Fig. 5 Peak heights of the spray-dried products at different

inlet gas temperatures.

Table 2 Average peak heights of the spray-dried products at different inlet gas temperatures. [Change in moisture content, % (100 kg kg1 dry basis).].

210

220

food and bioproducts processing 8 7 ( 2 0 0 9 ) 8795

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food and bioproducts processing 8 7 ( 2 0 0 9 ) 8795

Fig. 6 Mass spectra of raw (top) and spray-dried (bottom) sucrose in the positive ion mode.
for lower inlet gas temperatures and lower liquid ow rates.
However, the outlet gas temperature does not collapse the
curves in Figs. 3 and 4 to a noticeable extent, suggesting that
the temperature-time history of the particles throughout the
dryer may be important, as included in the model by Chiou et
al. (2008a).
Nevertheless, Table 2 shows that the sorption peak heights
(a measure of the degree of crystallinity) for sucrose can be
altered from less than 1% to about 20% (based on these sorption test results) depending on the pump (liquid ow) rate,
which is signicant compared with the alteration found for
lactose from around 8 to 9% (Chiou et al., 2008a). As expected,
the change in crystallinity for sucrose is higher than that for
lactose for a similar range of inlet gas temperatures, due to
the lower glass-transition temperature for sucrose that gives
greater scope for changing the difference between the material temperature and the glass-transition temperature in this
spray dryer.

3.3.
Assessment of the degree of thermal degradation
for spray-dried sucrose
Two samples of sucrose (raw sucrose and spray-dried sucrose)
were analyzed for degradation products that could have
resulted from the processing by spray drying. Three analytical
tests (Liquid ChromatographyMS, FTIR, Ion Chromatography)
were performed to assess the product composition and degradation of powders produced at an inlet gas temperature of
220 C and a 3% pump rate. Simple sugars form complex

degradation products upon heating at aerobic and anaerobic conditions, in a process called caramelization (Jiang et al.,
2008). Caramelization is the process of removal of water from
a sugar molecule, followed by isomerization and polymerization steps. The polymerization products are very complex
and poorly dened compounds with high molecular weights
and a system of conjugated double bonds responsible for the
characteristic dark brown color of thermally dehydrated sugar
molecules.
LCMS mass spectra of the two samples were obtained by a
ow injection using a mobile phase of 80% CH3 CN and 20% H2 O
(data not shown). A strong sodiated adduct ion was observed
in the positive mode (Fig. 6) but only a low intensity negative
sucrose ion was detected in the negative mode (Fig. 7). Ammonium acetate (10 mM CH3 COONH4 ) was added to water, and
this signicantly increased sucrose ionization in the negative
mode, where a strong deprotonated peak was observed with
an m/z of 341.2 and a dimmer with m/z of 683.4. No additional
peaks with higher m/z ratios were observed for the spray-dried
sample, indicating the absence of product degradation.
Ion Chromatography (IC) tests were performed for the
spray-dried sucrose samples to assess the purity. According to
the analysis, no detectable presence of degraded sugar units
was found.
Two virtually identical spectra were obtained from the FTIR
analysis of raw and spray-dried sucrose (Fig. 8). This suggests
that no new functional group(s) were formed, and there was
no evidence for any breakage of existing chemical bonds in
the case of spray-dried sucrose.

food and bioproducts processing 8 7 ( 2 0 0 9 ) 8795

93

Fig. 7 Mass spectra of raw (top) and spray-dried (bottom) sucrose in negative ion mode.

The MDSC results also suggest that both the raw sucrose
and the dried sucrose at these conditions were very crystalline
in nature, by showing similar melting curves (heat of melting
102.9 J/g and 100.0 J/g for spray-dried and raw sucrose powders, respectively) in the thermographs (Fig. 9). There were
no indications of glass transitions, and crystallization due to
amorphicity of the powders in the thermograph obtained from
the MDSC analysis was absent (Fig. 9). This proves the very
similar nature of the raw and spray-dried sucrose powders in
terms of their crystallinity.
The test results from all these methods are in good agreement and conrm that the sucrose dried at these operating

Fig. 9 MDSC of raw and spray-dried sucrose.

conditions did not break down into smaller carbohydrate

molecules (smaller sugar units) and was not converted into
other sugar polymers (like caramel) to any signicant extent
(undetectable and certainly less than 1% from the instrument
sensitivity).

3.4.

Fig. 8 ATR-FTIR of raw and spray-dried sucrose.

SEM micrographs

The surface morphology in the following micrograph also conrms the crystallinity of the powders produced at an inlet gas
temperature of 220 C and a 3% pump rate (Fig. 10).

94

food and bioproducts processing 8 7 ( 2 0 0 9 ) 8795

Fig. 10 Sucrose powders produced at inlet gas temperature of 220 C and a 3% pump rate.

4.

Conclusions

Stickiness of sucrose and sugar-rich materials at higher processing conditions has been an issue not allowing those
products to be spray dried on an industrial scale, because of
low yield. It has been found that very large changes in the
degree of crystallinity for the nal spray-dried product can be
achieved for sucrose by using different inlet gas temperatures,
compared with much smaller changes in the crystallinity of
lactose for a similar range of inlet temperatures. This result
supports the suggestion that the crystallization rate is related
to the difference between the material temperature and the
glass-transition temperature. Therefore, with materials having low glass-transition temperatures, such as sucrose, the
yield from spray drying can be signicantly increased by
processing the materials at sufciently high inlet gas temperatures without necessarily degrading the products signicantly,
through crystallizing the materials within the dryer.

References
Aguilera, J.M., Valle, J.M.D. and Karel, M., 1995, Caking
phenomena in amorphous food powders. Trends in Food
Science and Technology, 6(5): 149155.
Bhandari, B.R., Datta, N., Crooks, R., Howes, T. and Rigby, S.,
1997a, A semi-empirical approach to optimise the quantity
required to spray dry sugar-rich foods. Drying Technology,
15(10): 25092525.
Bhandari, B.R., Datta, N. and Howes, T., 1997b, Problems
associated with spray drying of sugar-rich foods. Drying
Technology, 15(2): 671684.
Bhandari, B.R. and Howes, T., 1999, Implication of glass transition
for the drying and stability of dried foods. Journal of Food
Engineering, 40(12): 7179.
Buckton, G. and Darcy, P., 1996, Water mobility in amorphous
lactose below and close to the glass transition temperature.
International Journal of Pharmaceutics, 136(1-2): 141146.
Buera, M.D.P. and Karel, M., 1993, Application of the WLF equation
to describe the combined effects of moisture and temperature
on nonenzymatic browning rates in food systems.Pdf. Journal
of Food Processing and Preservation, 17(1): 3145.
Busin, L., Mortazavi, F. and Bimbenet, J.-J., 1995, Spray drying of
sugar solutions. Industries Alimentaires et Agricoles, 112(78):
485489.
Champion, D., Meste, M.L. and Simatos, D., 2000, Towards an
improved understanding of glass transition and relaxations in
foods: molecular mobility in the glass transition range. Trends
in Food Science & Technology, 11(2): 4155.
Chiou, D., Langrish, T.A.G. and Braham, R., 2008a, The effect of
temperature on the crystallinity of lactose powders produced
by spray drying. Journal of Food Engineering, 86(2): 288293.

Chiou, D., Langrish, T.A.G. and Braham, R., 2008b, Partial

crystallisation behaviour during spray drying: simulations
and experiments. Drying Technology, 26(1): 2738.
Gordon, M. and Taylor, J.S., 1952, Ideal copolymer and the
second-order transition of synthetic rubbers. I Non-crystalline
copolymers. Journal of Applied Chemistry, 2: 493500.
Hanus, M.J. and Langrish, T.A.G., 2007, Re-entrainment of wall
deposits from a laboratory-scale spray dryer. Asia-Pacic
Journal of Chemical Engineering, 2(2): 90107.
Imtiaz-Ul-Islam, M. and Langrish, T., 2008, The effect of the salt
content on the crystallization behaviour and sorption
ngerprints of spray-dried lactose. Food and Bioproducts
Processing, 86(4): 304311.
Jiang, B., Liu, Y., Bhandari, B. and Zhou, W., 2008, Impact of
caramelization on the glass transition temperature of several
caramelized sugars. Part I: chemical analyses. Journal of
Agricultural and Food Chemistry, 56(13): 51385147.
Langrish, T.A.G., 2008. Degradation of vitamin C in spray dryers
and temperature and moisture content proles in these
dryers, Food and Bioprocess Technology, available online,
doi:10.1007/s11947-007-0039-5, in press.
Lehto, V.-P., Tenho, M., Vh-Heikkil, K., Harjunen, P.,
Pllysaho, M., Vlisaari, J., Niemel, P. and Jrvinen, K., 2006,
The comparison of seven different methods to quantify the
amorphous content of spray dried lactose. Powder
Technology, 167(2): 8593.
Levine, H. and Slade, L., 1986, A polymer physico-chemical
approach to the study of commercial starch hydrolysis
products. Carbohydrate Polymers, 6(3): 213244.
Meste, M.L., Champion, D., Roudaut, G., Blond, G. and Simatos, D.,
2002, Glass transition and food technology: a critical
appraisal. Journal of Food Science, 67(7): 24442458.
Ozmen, L. and Langrish, T.A.G., 2003, An experimental
investigation of the wall deposition of milk powder in a
pilot-scale spray dryer. Drying Technology, 21(7):
12531272.
Paterson, A.H.J., Brooks, G.F., Bronlund, J.E. and Foster, K.D., 2005,
Development of stickiness in amorphous lactose at constant
T Tg levels. International Dairy Journal, 15(5): 513519.
Rahman, M.S., 2006, State diagram of foods: its potential use in
food processing and product stability. Trends in Food Science
& Technology, 17(3): 129141.
Roos, Y., 1993, Melting and glass transitions of low molecular
weight carbohydrates. Carbohydrate Research, 238: 3948.
Roos, Y. and Karel, M., 1990, Differential scanning calorimetry
study of phase transitions affecting the quality of dehydrated
materials. Biotechnology Progress, 6(2): 159163.
Roos, Y. and Karel, M., 1991a, Amorphous state and delayed ice
formation in sucrose solutions. International Journal of Food
Science and Technology, 26(6): 553566.
Roos, Y. and Karel, M., 1991b, Plasticizing effect of water on
thermal behavior and crystallization of amorphous food
models. Journal of Food Science, 56(1): 3843.
Roos, Y. and Karel, M., 1992, Crystallization of amorphous lactose.
Journal of Food Science, 57(3): 775777.

food and bioproducts processing 8 7 ( 2 0 0 9 ) 8795

Schenz, T.W., 1995, Glass transitions and product stabilityan

overview. Food Hydrocolloids, 9(4): 307315.
Senoussi, A., Dumoulin, E.D. and Berk, Z., 1995, Retention of
diacetyl in milk during spray-drying and storage. Journal of
Food Science, 60(5): 894897.
Slade, L. and Levine, H., 1994, Water and the glass
transition-dependence of the glass transition on composition
and chemical structure: special implications for our
functionality in cookie baking. Journal of Food Engineering,
22(14): 143188.

95

Soesanto, T. and Williams, M.C., 1981, Volumetric interpretation

of viscosity for concentrated and dilute sugar solutions.
Journal of Physical Chemistry, 85(22): 33383341.
Williams, M.L., Landel, R.F. and Ferry, J.D., 1955, The temperature
dependence of relaxation mechanisms in amorphous
polymers and other glass-forming liquids. Journal of the
American Chemical Society, 77(14): 37013707.
Wise, C.W., Cook, W.D. and Goodwin, A.A., 1997,
Chemico-diffusion kinetics of model epoxy-amine resins.
Polymer, 38(13): 32513261.