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00
q Institution of Chemical Engineers
Trans IChemE, Vol 76, Part C, March 1998

HEAT TRANSFER IN TWO-PHASE SOLID-LIQUID

FOOD FLOWS: A REVIEW
M. BARIGOU, S. MANKAD* (GRADUATE) and P. J. FRYER (FELLOW)
School of Chemical Engineering, University of Birmingham, Birmingham, UK
*Department of Chemical Engineering, University of Cambridge, Cambridge, UK

H
igher quality food can be produced by continuous aseptic processes rather than by the
essentially batch process of in-container sterilization of particulate foods. In
continuous aseptic processing, a food mixture passes continuously through a heat-
hold-cool system, and is then packaged in presterilized containers. This results in shorter
processing times, higher production rates, superior product quality, reduced power
requirements, and improved process control. The design of such a plant requires knowledge
of the rates of heat exchange (both ¯ uid-particle and wall-¯ uid) which take place within the
process. At present there is a severe lack of understanding of two-phase solid-liquid food ¯ ows,
and suitable commercial sterilization schedules must be determined experimentally for every
food product processed. Until enough knowledge of real ¯ ows has been gained, food
manufacturers will adhere to conservative approaches in the design of each stage in a heat-
hold-cool system. Following the recent review on the ¯ uid mechanics of solid-liquid food
¯ ows6 , this paper reviews the current state-of-the-art in the area of heat transfer. The ¯ uid-
particle and the wall-¯ uid heat transfer coef® cients are crucial design parameters.
Measurement techniques and mathematical models for estimating them are reviewed, the
application of existing knowledge to the design of continuous aseptic processes is discussed,
and research needs are highlighted.
Keywords: aseptic processing; food sterilization; heat transfer coef® cient; mathematical
modelling; particulate food; solid-liquid ¯ ow

The processes which result in quality loss have a lower

1. INTRODUCTIO N
Cooking represents a critical step in most food manufactur-
ing processes. Thermal processing brings about irreversible
changes in food textural and sensoric properties, whilst at
the same time achieving the desired level of microbial
sterility. It is not possible nor is it necessary to eliminate all
viable organisms from the material. Organoleptic and
nutritive properties of foods are adversely affected by
heat, and the process must only be as severe as necessary to
ensure commercial sterility. Spore reduction and nutrient
loss are governed by different kinetics, the rates of which
are dictated by the processing conditions. A food that is
optimally cooked would be safe but would also have
sensoric and nutritious properties that are most acceptable to
the consumer. The optimization of such thermal treatments
poses a challenging manufacturing problem. The overriding
importance of food safety often results in the food being
exposed to a more severe process than is desirable from a
quality aspect, resulting in lower sensoric and nutritional
attributes, especially with sensitive products, than is
actually possible. Without con® dence in the design data,
processes will always be overdesigned for safety.
The problem of optimizing such a process is dif® cult for
single phase foods; it is even more intractable when
inhomogeneous highly-viscous foodstuffs bearing large
solid food particulates are handled.
activation energy than those which result in sterility1 . At
high temperatures, sterilization reactions proceed about 100
times faster than loss of quality reactions: the time needed
for sterilization is reduced and the amount of quality loss is
also reduced. Hence, there is a clear quality advantage in
sterilizing at higher temperatures and for shorter times i.e.
HTST2 . HTST processes involve heating to temperatures in
the region of 1408 C for about 10 seconds, holding the
product at the sterilization temperature for long enough to
ensure suf® cient pathogen spore destruction, and then
cooling to packaging temperature. Rather than the essen-
tially batch process of canning, the HTST process requires
the product to pass continuously through the system at high
¯ owrates to optimize productivity; this necessitates inde-
pendent sterilization of the product and package, and is
termed aseptic processing.
The literature on the thermal processing of foods is
obviously enormous: here, the focus is on the continuous
aseptic processing of food products consisting of both
viscous liquid and (large) solid constituents. This is being
increasingly considered as a better substitute for traditional
heat treatment in containers3 . Higher production rates,
improved product quality because of relatively short heating
and cooling times, reduced energy requirements, and more
amenability to automatic control are all attractive features of
continuous aseptic processing. The process in its essential

3
4 BARIGOU et al.
form consists of pumping the solid-liquid food mixture
through a heat exchanger. If this heat exchanger is a
conventional one, using convective heat transfer, most of
the heat goes only into the liquid as the residence time in the
heat exchanger is short and the rate of transient-conduction
heat transfer inside the particle is low. Therefore, little more
than a steep temperature gradient from the outside to the
centre of the particle will have been established by the time
the particle exits the heat exchanger. The mixture then
passes into an insulated holding tube where suf® cient time is
given for the solid particles to be indirectly heated by the
liquid to the desired level. From here, the food passes into
one or more heat exchangers where it is cooled prior to
packaging: here the particle temperature will often be
greater than the surrounding liquid. For example, in the
APV ohmic-heaterprocess4 ,5 , between 100and1000 kghr- 1 of
food mixtures containing 50% solids up to 25 mm in
diameter, are pumped through pipes of 0.075- 0.15 m
diameter, i.e. at average ¯ ow velocities on the order of
0.1 ms- 1 .
The technology has been successfully applied to single
phase liquid foods. Its widespread application to food
products containing both liquid and solid constituents is
severely limited by the lack of understanding of the
principles that govern the transfer of heat within such
foods as they ¯ ow through the processing equipment. The
often complicated rheology of the foods which usually
consist of a highly viscous non-Newtonian liquid carrying
almost neutrally-buoyant solid food pieces, causes the
¯ ow through the equipment to be non-uniform and often
unpredictable6 . The process may thus be subjected to a
wide distribution of particle concentration, velocities,
residence times, and temperatures, thereby causing a wide
and still largely unpredictable distribution of those
quality changes that are imparted to the food by the
heat treatment. The problem is distinct from that of
processing packaged foods, which is discussed in detail
by Holdsworth7 .
In conventional heat transfer, the processes which lead to
the heating of particles are:
(i) transfer of heat from some external source to the
exchanger surface;
(ii) transfer from the exchanger wall to the ¯ uid,
characterized by a wall heat transfer coef® cient, hw ;
(iii) convective mixing or conduction through the particle-
¯ uid mixture to the particle;
(iv) transfer from ¯ uid to particle, characterized by a
particle-¯ uid heat transfer coef® cient, hfp ;
(v) thermal conduction within the particle.
A successful design of a continuous heat-hold-cool
aseptic process for particulate foods couples safety
assurance with quality optimization. The absolute aim is
to ensure that the process delivers the necessary microbial
lethality to the slowest heating zones within the particles
whilst not over-processing any signi® cant amounts of the
product. Factors in¯ uencing process design are of three
principal categories:
(i) Heat Transfer
In addition to design considerations for processing
liquids, there are a number of extra parameters associated
with food particle heating which directly affect the design of
equipment used to process liquids with particles1 ,8 ± 1 0 ,
(a) particle sizeÐ the larger the particle the harder it is to
sterilize;
(b) particle shapeÐ different shapes lead to different rates
of heat transfer to the particle centre;
(c) particle thermal propertiesÐ density, speci® c heat
capacity, and thermal conductivity which has the most
important effect on particle centre heating;
(d) convective heat transfer coef® cient at particle surface
(hf p )Ð this is a vital parameter for estimating the steriliza-
tion rate at the geometric centre of the particle, but at the
same time it is very dif® cult to measure. As shown in
Table 1, many workers have developed dimensionless
correlations for predicting hf p of the form: Nu = a+
bRec Prd , where, for a single isolated particle, the limiting
Nusselt number usually corresponds to a = 2. Attention
must be paid to the de® nition of the Reynolds number as
different forms of Re are found; and
(e) heat transfer coef® cient between the two-phase mixture
and the pipe wall (hw )Ð which has been much less well
studied than hfp , but could well be as signi® cant1 1 . This
parameter has usually been estimated by assuming either
laminar or turbulent ¯ uid ¯ ow in the pipe, or assuming
an arbitrary high value (, 1000 Wm- 2 K- 1 )1 2 .
Another aspect that should be considered in the design is
the contribution of the cooling stage to product sterilization.
The centroids of the particles leaving the holding tube will
cool at a ® nite rate and some reaction leading to microbial
lethality must occur. Conservative approaches tend to
ignore this contribution. An optimal process design should
take into account all contributions to lethality from the
heating, holding and cooling stages.
(ii) Particle and Liquid Flow
In a recent review, Lareo et al.6 discussed outstanding
issues in the ¯ uid mechanics of solid-liquid food ¯ ows. The
microbiological lethality delivered to the particles and the
degree to which quality is maintained is a function of the
residence time of the particles in the process as well as the
temperatures. This must be taken into account when
establishing a continuous heat preservation process. The
factors affecting particle residence time are:
(a) particle size Ð most food products contain a range of
particle sizes, which in¯ uences particle ¯ ow behaviour.
Particle size together with the properties of the liquid carrier
affect the residence time; over the last ten years some
workers have begun to study particle residence time
distributions1 3 ± 1 5 ;
(b) velocity pro® le of the carrier liquid within the ¯ ow
channelÐ the residence time of a particle will depend on its
radial location within the conveying liquid;
(c) particle concentration pro® le which is usually non-
uniform with a minimum at the wall;
(d) the heat exchanger con® guration, which will affect the
¯ ow ® eld and, thus the particle residence time. For example,
the ¯ ow pro® le through the barrel of a scraped surface heat
exchanger is far more complex than that through a straight
tubular heat exchanger1 6 . On the other hand, the presence of
Trans IChemE, Vol 76, Part C, March 1998
 HEAT TRANSFER IN TWO-PHASE SOLID-LIQUID FOOD FLOWS
® ttings and especially the presence of multiple turns in
holding tubes is likely to prevent the establishment of
a stable velocity pro® le and in consequence affect the
particle residence time distribution. A good process design
should aim at achieving a narrow particle residence time
distribution.
A continuous heat sterilization process usually has two
critical control points1 0 : (i) monitoring of the largest particle
in the product as it has the slowest heating rate at its centre,
and on which the design of the process must be based; and
(ii) estimation of the shortest particle residence time in the
process. The latter is a far more complex critical control
point as particle residence time is poorly understood. In
general, much remains to be learned about the dynamics of
food particles conveyed by a viscous liquid in a continuous
aseptic process.
(iii) Quality Optimization
The complexity of designing an aseptic process for
maximum product quality is similar to that of optimizing
microbial lethality; both are limited by the lack of knowl-
edge and control of particle ¯ ow and the associated
residence time distribution. When designing for optimum
product quality, account must be taken of the temperature
history in the carrier liquid as well as within the particles.
The degree of product quality expected from the process can
only be estimated by integrating these two temperature-time
histories for the phases together with appropriate kinetic
parameters for quality: few studies1 7 have examined this
important problem.
The type and layout of the process poses a further barrier
to quality optimization. In a continuous system, ® nal
product quality will be a direct consequence of the ability
of the process to achieve truly HTST sterilization. For
optimum product quality, the time to heat the particle
centroids to the required temperature, to hold them at this
temperature, and then to cool them, must be minimized, and
all stages of the process must be optimized. The design of
the equipment affects both particle residence time and heat
transfer rates, and hence the ® nal product quality. Appro-
priate equipment must, therefore, be chosen with regard for
optimum quality. Increasing consumer demands for better
quality may well stimulate the development of novel
designs; for example, some solutions have been suggested,
such as the ohmic heater in which heat is generated within
particles by the passage of electric current, obviating the
need for heat transfer during the heating stage (see for
example Zhang and Fryer1 8 ; Fryer1 9 ). This, however, does
not eliminate the need for effective coolingÐ indeed, since
particles can heat faster than the surrounding ¯ uid during
ohmic heating, cooling can be more important to product
quality here.
At present, a suitable commercial sterilization schedule
must be established experimentally for every food product
processed. It is likely that food manufacturers will adhere to
this approach in the design of each stage in a heat-hold-
cool system. However, without an understanding of the
design factors, processes will be set so that products are
over-processed to ensure safety. The damage to delicate
particulates resulting from over-processing will restrict the
range of food products that could bene® t from continuous
Trans IChemE, Vol 76, Part C, March 1998
5
aseptic processing technology; the consumer will not pay
extra unless products are demonstrably better. The FDA
have recently approved an aseptic process involving par-
ticulates1 1 8 ; the use of data and models is to enable processes
which fully exploit the advantages of continuous processing.
This paper reviews the current state-of-the-art in the area
of heat transfer in two phase solid-liquid ¯ ows. The
application of existing knowledge to the design of
continuous processes for the heat treatment of particulate-
bearing food systems is discussed, and research needs
highlighted.
2. FLUID-PARTICLE HEAT TRANSFER
The in¯ uence of the surface heat transfer coef® cient, hf p ,
on the thermal response of a particle will vary; for large
particles internal thermal conduction is the controlling (i.e.
slowest) process, so that varying hfp does not affect the
process time. The particle Biot number, Bi, compares the
heat transfer rates resulting from external heat transfer and
internal thermal conduction, and thus gives a measure of the
mechanism which controls the rate of heating. It is de® ned
as
hfp x
Bi = (1)
ks
where ks is the particle thermal conductivity, and x is a
characteristic dimension of the particle. For spheres, for
which x is the radius, if Bi < 0.1 the conductive resistance in
the solid is small and hf p controls the thermal behaviour,
whilst if Bi > 10 the convective resistance is small i.e. hf p is
large and heat transfer is conduction controlled2 0 . Between
these two values a combination of mechanisms controls heat
transfer. In the limit when Bi ! 0, the particle will be
isothermal and heat transfer solely controlled by external
factors; for this case the problem has an exact analytical
solution known as Newton’ s law of heating,
mp Cp Tp - Tf
Ap
ln
Ti - Tf = - hfp t, (2)
which gives the temperature change when a particle of mass
mp , surface area Ap , and speci® c heat capacity Cp , is heated
from temperature Ti to Tp , for time t, in a ¯ uid at constant
temperature Tf .
Published research has adopted two different approaches
to determine hf p . Both use a transducer particle with a
known Biot number; the convective heat transfer coef® cient
can be estimated from the temperature history of the
particle. The two approaches are to use particles where: (i)
Bi = 0, assuming the entire particle volume is at constant
temperature and then evaluating the heat transfer coef® cient
from equation (2) or its equivalent for non-uniform ¯ uid
temperature; and (ii) Bi Þ 0, in which the transient heat
conduction equation (18a) must be solved to obtain hf p . The
latter approach can be inaccurate, as particle heating rate
becomes increasingly insensitive to hf p as Bi increases, i.e.
as thermal conductivity controls, so data for hf p ® tted from
experiments with high Bi particles may be worse than from
low Bi experiments.
Data has been commonly expressed in terms of correla-
tions relating Reynolds, Prandtl and Nusselt numbers. The
velocity that controls the interfacial heat transfer will be the
 6
Table 1. Convective heat transfer coef® cients for particles in continuous ¯ ow.

Particle shape Reynolds

and size hfp number Experimental
Reference (mm) Carrier ¯ uid (Wm- 2 K- 1 ) range Pr Nu Correlation method

Baptista et al.105 sphere CMC Thermocouple

1.27±2.23 (0.10±0.60%)
(aluminium) w/w)
stationary 56±2612 4.1 < Rep < 636 69±1810 9.0±88.3 Nus = 2 + (0.025 6 0.004)Prs1/ 3 Gr 1/ 2 ; 2.8 < Gr < 4840
.676 0.03)Pr (0.386 0.03)
Nu = Nus + (0.20 6 0.06)Re(0 p s
(0.706 0.04) (0.426 0.06)
rotating 67±1782 0.1 < Rep < 801 71±5340 2.5±60.7 Nu = Nus + (0.081 6 0.04)Rep Prs
.716 0.03)Pr (0.426 0.04)
Nu = Nus + (0.17 6 0.06)Re(0 p s
dp (0.286 0.05)
´ d
t
` Nus : Nusselt number for natural convection and
non-Newtonian ¯ uid
Prs : generalized Prandtl number for zero ¯ uid velocity,
based on intrinsic viscosity.

Mankad et al.36 sphere water ± 292 < Rep < 2433 ± 20±60 Nu = 2 + 1.41Re0p.47 Thermocouple
15
(copper) polyacrylamide ± 114 < Rep < 893 ± 20±48 Nu = 2 + 3.20Re0p.38
(0.5% w/w)
glycerol:
67% w/w ± 18 < Rep < 140 ± 16±36 Nu = 2 + 4.98Re0p.39
83% w/w ± 5 < Rep < 97 ± 9±34 Nu = 2 + 5.67Re0p.49
for all ¯ uids used: Nu = 2 + 0.97Re0p.45 Pr0.25
BARIGOU et al.

1.441
dp
Gadonna et al.75 sphere water 290±466 1400±2300 ± 4.87±13.42 Nu = 2 + 4.98Re0.234 Liquid crystal
9.1±24.0 dt
(polypropylene)
dp 2.217
346±1587 2300±5000 ± 5.33±45.72 Nu = 2 + 19.31Re0.279
dt
290±1587 2300±5000 ± 4.87±45.72 Nu = 2 + 0.0933Re0p.727 ; 84 < Rep < 2300
dp 0.514
Nu = 2 + 0.228Re0p.639 ; 84 < Rep < 2300
dt
Nu = 2 + 14.44Frp0.777 ; 0.177 < Frp < 1.714
dp 1.99
Nu = 2 + 129.35Frp0.712 ; 0.177 < Frp < 1.042
dt

Kelly et al.27 cube: 10.0±32.0 water ± 239 < Rep < 5012 2.3±4.3 14±76 Nu = 0.298Re0p.62 Pr0.36 Thermocouple
sphere: 9.5±30.0 Nu = 2.0 + 0.206Re0p.66 Pr0.39 (open channel
cylinder: dp = 12.7± ¯ ow)
32.5; l = 12.8±31.9
(aluminium) CMC ± 4.5 < Rep < 177 0.02±0.14 17±53 Nu = 21.13Re0p.12 Pr- 0.076
(0.8±1.5% w/w) Nu = 2.0 + 19.36Re0p.132 Pr- 0.08

Trans IChemE, Vol 76, Part C, March 1998

 Table 1. (Continued)

Particle shape Reynolds

and size hfp number Experimental
Reference (mm) Carrier ¯ uid (Wm- 2 K- 1 ) range Pr Nu Correlation method

A
ÊstroÈm and sphere, cube silicone oil, 110±450 ± ± ± Nu = 8 + 2.53Re0.54 ; particle at 50 mm from axis Thermocouple
Bark48 8±16 starch (6% w/w) of rotation. (stationary
(lead) Nu = 8 + 2.25Re0.61 ; particle at 11 mm from axis particle in a
of rotation. rotating ¯ uid)

Balasubraniam Sphere CMC ± ± Thermocouple

and Sastry34 12.8±22.3 (0.2, 0.5, 363±2010 0.0058±798 104.5±2443 Liquid crystal
0.8% w/w) 1 < Rep < 193 Relative velocity

Awuah et al.115 cylinder: CMC Thermocouple

dp = 16.0±23.0; (0.5, 1% w/w)
l = 22.3-40.0

Trans IChemE, Vol 76, Part C, March 1998

carrot 80±456 ± 1.23±7.02 ± Nu = 2.45(PrGr)0.108 ; 0.1 ´ 104 < Gr < 10.96 ´ 104
potato 100±556 ± 1.23±7.02 ± Nu = 2.02(PrGr)0.113 ; 0.11 ´ 104 < Gr < 11.1 ´ 104

Bhamidipati and cylinder CMC ± 0.310±1.687 1.32± 5.12±9.26 Nu = 0.27Re0p.2 Pr0.33 Remote
Singh106 dp = 10.7; 0.5±1.2% w/w 4.73 ´ 104 temperature
l = 22.6 sensor

Damay and Pain76 sphere dp 1.221

19.4±26.3a water 990±2260 8950±22000 ± ± Nu = 2 + 0.092Re0.76 Melting point
dt indicator
19.0±26.0b 1460±3346 8000±24000 ± ± Nu = 2 + 0.225Re0.626
Nu = 2 + 1.221Re0.432 Frp0.163
Material with dp 0.88
change of phase at Nu = 2 + Re0p.52
a b dt
- 128 C and 08 C .

Mwangi et al.35 Sphere glycerol ± 563±6000 3.68±5.52 ± Laminar: Nu = 0.10Re0.58 Pr 0.33 Melting point
8±12.7 (19, 21, 23% Turbulent: Nu = 0.0336Re0.80 Pr0.32 indicator
w/w)
HEAT TRANSFER IN TWO-PHASE SOLID-LIQUID FOOD FLOWS

Zuritz et al.28 mushroom CMC dp 1.787 Thermocouple

20.6±28.2 548±1175 0.123±1.94 1.14±7.22 17.2±50.29 Nu = 2 + 28.37Re0.233 Pr0.143
(aluminium) dt
dp : diameter of projected cap perimeter
7
 8
Table 1. (Continued)

Particle shape Reynolds

and size hfp number Experimental
Reference (mm) Carrier ¯ uid (Wm- 2 K- 1 ) range Pr Nu Correlation method

Chandarana et al.69 cube water 64.7±107.11 287.3±880.7 ± ± Nu = 2.0 + 0.0333Re1.08 Thermocouple

(silicone)
1 .6
starch 55.63±89.5 1.23±27.38 9.5±376.2 ± Nu = 2.0 + 0.0282Re Pr 0.89
(2±3% w/w)

Sastry et al.46 sphere water 688±3005 3600±27300 ± ± Nu = 26.81 + 0.00455Re(dp / dt ) Moving

13.3±23.9 Nu = 6.023x10- 6 Re1.79 (dp / dt )1.71 Fr- 0.64 thermocouple
(aluminium) Nu = 0.046Re + 41.54(dp / dt ) - 35.65Fr - 5.42
Nu = 0.125Re + 85.67(dp / dt ) - 342.5Fr
- 0.0144Re(dp / dt ) + 0.0113ReFr
+ 500.3Fr(dp / dt ) - 0.0173ReFr(dp / dt )
- 26.56.
Fr = 0.39 - 14.83; dp / dt = 0.2618 - 0.6273

Incorpera and ¯ at plate ± ± ± ± ± Nu = 0.332Re0.5 Pr0.33 ±

De Witt109

Chandarana et al.26 cube water 65.67±107.11 761±2144 ± ± Nu = 0.85Re0.434 Thermocouple

(silicone)
starch 55.63±89.5 5.6±141.8 40.8±1564 ± Nu = 0.55Re0.438 Pr 0.349
(2±3% w/w)
BARIGOU et al.

Zuritz et al.68 mushroom CMC 548±1175 0.11±2.00 1.05±8.36 ± Nu = 2 + 7.9464Re0.20795 Pr0.14413 Thermocouple
(aluminium) Nu = 22.7 + 0.036Re0.45 Pr0.53

Heppell25 Sphere water 2180±7870 5250±50000 ± 110.8±400.2 ± Biological

3
starch 930 30 ± ± ±
5% w/w

Chuchottaworn107 ± ± ± ± ± ± Nu = 2.0 + 0.37Re0.61 Pr0.51 ±

Whitaker 67 sphere air, oil, water ± 3.5 ´ 104 < Rep 0.71±380 l 0.25
<7.6 ´ 104 Nu = 2.0 + (0.4Re1/p 2 + 0.06Re2/p 3 )Pr0.4 ±
l p

Noordsij and sphere water ± 400-1350 500±2000 ± Nu = 10 + 0.608Re1/w 2 Pr 1/ 3 ±

Rotte112 (nickel) initially obtained for mass transfer

Trans IChemE, Vol 76, Part C, March 1998

 Table 1. (Continued)

Particle shape Reynolds

and size hfp number Experimental
Reference (mm) Carrier ¯ uid (Wm- 2 K- 1 ) range Pr Nu Correlation method

Ranz and liquid drop air ± 1 < Rep < 104 0.6±400 ± Nu = 2.0 + 0.6Re0p.5 Pr 0.33 Evaporation
Marshall66 0.6±1.1 from pure liquid
drops

Kramers65 sphere air, oil, water ± Rep < 105 0.7±400 10±400 Nu = 2.0 + 1.3Pr0.15 + 0.66Pr 0.31 Re0p.5 ±
(steel)

Williams114 sphere ± ± >200 ± ± Nu = 0.37Re0.6 Pr0.33 ±

Johnstone et al.110 sphere ± ± >500 ± ± Nu = 0.714Re0.5 Pr 0.5 ±

Ljachowski111 sphere (metal) air ± 200±30000 ± ± Nu = 0.61Re1/ 2 ±

Trans IChemE, Vol 76, Part C, March 1998

sphere (steel,
mercury) water ± 3500±15000 ± ± Nu = 0.085Re0.78 ±

Vyroubow113 sphere air ± 200±3000 ± ± Nu = 0.58Re1/ 2 Pr 1/ 3 ±

(metal)

FroÈszling108 sphere air ± 2±800 0.6±2.7 ± Nu = 2.0 + 0.55Re1/ 2 Pr 1/ 3 ±

(water,
nitrobenzene,
aniline,
naphthalene)
HEAT TRANSFER IN TWO-PHASE SOLID-LIQUID FOOD FLOWS
9
10 BARIGOU et al.
relative velocity between particle and ¯ uid (i.e. the slip
velocity); some correlations do not include this but use the
overall velocity instead. However, the slip velocity in real
mixtures is often not known and may be dif® cult to de® ne.
To de® ne slip as the difference between the mean ¯ uid
velocity and particle velocity is not complete, because of the
complexity of the ¯ ow and the liquid velocity gradient. For
example, several workers including Lareo1 5 have found that
particles in a viscous carrier ¯ uid travel faster than the mean
¯ uid velocityÐ this arises because particles congregate
into the centre of the ¯ ow where the liquid is fastest.
Experiments in a well-de® ned ¯ ow ® eld may thus give
correlations in terms of a slip Reynolds number that cannot
be estimated for a real system. Conversely, whilst experi-
ments in real ¯ ows give actual hfp data, the ¯ ow ® eld which
produces them is not known. Figure 1 shows some existing
results for forced convection heat transfer. The data were
calculated from cases where correlations were given in
terms of the particle-¯ uid slip velocity; hence, this plot
excludes data such as that of Sastry et al.2 1 where the
correlations were not derived in terms of slip velocity. All
correlations are plotted for water at 158 C (Pr = 7.425) so
that the correlations may be compared on the same basis.
This graph shows that data are scattered over a wide range
of Nusselt numbers, and there is no clear association
between the different sets of data. This may be due to a
number of effects including: (i) experimental inaccuracies,
such as the presence of natural convection at low Re; (ii)
discrepancies in the real velocity ® eld experienced by the
particle, where the slip quoted is not representative of the
¯ ow ® eld around the particle; and (iii) different measure-
ment techniques.
2.1. Factors Governing Fluid-Particle Heat Transfer
Results for some of the main investigations on ¯ uid-
particle heat transfer are summarized in Table 1, in terms of
correlations for Nusselt number. The correlations re¯ ect the
fact that the convective heat transfer coef® cient is
in¯ uenced by several factors (see for example, Hendrickx
et al.2 2 and Stoforos2 3 ):
Figure 1. Variation of Nusselt number with slip Reynolds number for
existing experimental data.
2.1.1. Fluid viscosity
The effect of viscosity is shown by the difference in hf p
values obtained for low viscous ¯ uids, e.g. water, and more
viscous ¯ uids, e.g. aqueous CMC solution. Lenz and Lund2 4
obtained lower hf p values in a 60% aqueous sucrose solution
than in water. Heppell2 5 determined hfp by measuring the
destruction of Bacillus stearothermophilus in calcium
alginate particles (3.4 mm dia.) ¯ owing through a holding
tube. For a 5% starch solution, heat transfer was so low that
twice the residence time (and thus holding tube length) was
needed to achieve the sterilization effect predicted for the
case of in® nite hf p , i.e. zero resistance to interfacial heat
transfer. Chandarana et al.2 6 measured greater hf p values for
water (65.67±107.11 Wm - 2 K- 1 ) ¯ owing past silicone
cubes than for starch solutions (55.63±89.5 Wm - 2 K- 1 )
over the same temperature range (133±1458 C). Kelly et
al.2 7 measured hf p using aluminium cubes (10.0±32.0 mm),
spheres (9.5±30.0 mm dia.) and cylinders (12.7±32.5 mm
dia.; 12.8±31.9 mm length) in open channel ¯ ow, using
water and aqueous CMC solutions (0.8, 1.0, 1.2, 1.5% w/w)
at 558 C, ¯ owing at velocities 8.7-41.2 mm/s. The particles
were stationary and had a thermocouple imbedded at their
geometric centre to monitor temperature. An increase in
¯ uid viscosity caused a signi® cant decrease in hf p for all
¯ ow velocities. Other researchers2 8 ± 3 1 also reported that hf p
increases with decreasing CMC concentration.
Results can be interpreted in terms of the particle
Reynolds number, preferably slip Reynolds number, rather
than just viscosity. Viscosity has a number of effects: it will
in¯ uence the ¯ uid velocity pro® le and ¯ ow regime within
the tube as well as the drag force on the particle, and thus the
particle-liquid slip.
2.1.2. Particle slip velocity
Differences in solid-¯ uid translational velocities will
increase interphase heat transfer rates; the relative linear and
rotational ¯ uid motion over the particle gives increased
forced convection, and thus enhanced heat transfer. Typical
slip velocities occurring in food ¯ ows are in the region1 5
of 0.1 to 1 cms- 1 , and can affect heat transfer signi® cantly.
For example, a single food particle of diameter 10 mm with
a slip velocity of 1 cms- 1 would, in water, have a Nusselt
number of 45, as estimated from the Ranz-Marshall
correlation, equation (7). This is a considerable enhance-
ment over the value Nu = 2, i.e. no slip, used in many
existing theoretical models. Particle slip velocity will be
similar to the sedimentation velocity.
The information reported in the literature suggests that
stationary particles in a ¯ ow usually have higher surface
heat transfer coef® cients than particles moving with the
¯ uid. If, however, the relative velocity between particle and
¯ uid is the same, the heat transfer coef® cient for a stationary
particle in a moving ¯ uid should be similar to that for a
particle moving within its carrier ¯ uid. Chang and Toledo3 3
reported an increase in hf p from 239 to 303 Wm - 2 K- 1 when
the slip velocity increased from 0.38 to 0.86 cms- 1 , for
stationary potato cubes in water, and a non-Newtonian
solution with 35% sucrose. The same trend was observed by
Balasubramaniam and Sastry3 4 for moving aluminium
spheres in continuous tube ¯ ow using CMC solutions.
They used three different techniques to measure hf p : moving
thermocouple, relative velocity, and liquid crystal; these are
described later. Other workers have reported similar
Trans IChemE, Vol 76, Part C, March 1998
 HEAT TRANSFER IN TWO-PHASE SOLID-LIQUID FOOD FLOWS
experimental ® ndings (see for example, Sastry et al.2 1 ;
Zuritz et al.2 8 ; Mwangi et al.3 5 ; Mankad et al.3 6 ). Data
correlations are thus often expressed in terms of the slip
Reynolds number, although this may be dif® cult to
determine in practice.
The importance of slip velocity was shown by Mankad
et al.3 7 , and Mankad and Fryer3 8 , who used a one-
dimensional theoretical model to compute sterilizer lengths
for various solid-liquid slip velocities and delivered solids
concentration for a ® xed ¯ ow rate. Changing the slip
velocity between solid and liquid, and thus hf p , affected the
required sterilizer length greatly, highlighting the need to
incorporate slip effects in process design. The heating tube
length was found to be a strong function of slip velocity.
2.1.3. Particle concentration and particle-particle
interactions
Particle concentration and particle-particle interactions
are the factors with the least understood effects on hf p .
Existing results for the canning process are often irreconcil-
able; for example, the experiments of Lenz and Lund2 4
showed a decrease in hf p with an increase in particle loading,
whereas Hassan 3 9 observed the opposite.
The in¯ uence of particle-particle interactions on ¯ uid-
particle heat transfer has not been studied in detail by either
food scientists or process engineers. Two effects may occur:
(i) localÐ particle-particle interactions can disturb the ¯ uid
streamlines locally, which will affect the ¯ ow ® eld around
successive particles and, depending on the Reynolds number,
may enhance the convective heat transfer coef® cient;
(ii) overallÐ where particle concentration is high, ¯ uid
channelling through particles can occur and can signi® -
cantly affect the heat transfer coef® cient in sections of the
mixture; in places higher, in places lower (see, for example,
Agarwal4 0 and Paterson et al.4 1 ).
Dutta and Sastry3 2 studied the velocity distribution of
polystyrene spheres (9.5 mm dia., 1044.5 kgm- 3 ) in CMC
solutions. Particle motion was videotaped; it was seen that
as well as particle collision, particle-particle interactions
also occur via a hydrodynamic attraction-repulsion due to
pressure changes in the inter-particle gap. This phenomenon
was previously observed by Davis et al.4 2 who showed the
existence of a signi® cant pressure pulse between approach-
ing particles in a liquid, which may cause particles to
deform before collision. Dutta and Sastry3 2 also observed
that particle concentration affected the interactions as
particle motion became restricted at high solids fractions,
and that particles can change velocity as a result of
interaction with others. They did not, however, study the
effect of particle interactions on hfp .
Mwangi et al.3 5 measured hf p in a holding tube using
a melting point indicator technique with polymethyl-
methacrylate transducer particles (dp = 8.0-12.7 mm; q p =
1021.36±1100.74kgm- 3 ) in aqueous glycerine (19, 21,
23% w/w; q f = 1020-1100kgm- 3 ). The value of hf p
increased by 80 to 200% when the solids fraction was
increased from a single particle to 3.2% w/w. This increase
was attributed to the disturbance of the ¯ ow ® eld around the
transducer particle caused by the presence of other particles,
especially at high Reynolds numbers, which led to the
thinning of the boundary layer around the particle.
The effect of wake formation behind a particle on hf p was
Trans IChemE, Vol 76, Part C, March 1998
11
studied by Kelly et al.2 7 and Mankad1 1 . Kelly et al.2 7
studied the effect of a sphere placed at a distance l upstream
from a spherical transducer particle in water (T = 588 C;
uf = 0.0275 ms- 1 ). The effect of varying the separation
distance l and the sizes of the two particles on hf p was
investigated. When both particles were of the same size
(11.9 mm dia.), or the particle upstream of the transducer
particle was smaller (18.8 mm upstream of 25.1 mm dia.
particle or 25.1 mm upstream of 30.0 mm dia. particle), as l
increased from zero to 4 mm hf p increased from that for the
isolated particle to a maximum, falling off gradually back to
its initial value at about l = 100 mm. When the particle
upstream was larger (25.1 mm upstream of 11.9 mm dia.
particle or 25.1 mm upstream of 9.5 mm dia. particle), hf p
decreased slightly as l increased to 4 mm then peaked to a
maximum at l = 50 mm, falling back to its initial value at
l = 100 mm. Particle wake effects are thus complex and
depend strongly on the relative sizes of the interacting
particles.
Little information exists on how much heat transfer can
be enhanced through particle-particle interactions in con-
tinuous ¯ ows. Multiple particle systems, however, have
been widely studied in the ¯ uidization literature (see, for
example, Agarwal4 0 ). Three main con® gurations are of
importance: particulate ¯ uidization where particles are not
in contact with each other and their distribution is due to
system hydrodynamics; packed beds where particles are in
mutual contact and their orientation, random or regular, is
set by the process; and distented beds where the particles are
® xed in a regular orientation but are not necessarily in
contact. For constant ¯ ow rate, heat transfer has been found
to increase in distented beds as voidage decreases 4 0 . At all
but very low Reynolds numbers, heat transfer coef® cients in
packed beds, which will have the most inter-particle
interactions, are considerably higher (approximately a
factor of 2.5-3) than heat transfer coef® cients for single
particles1 1 ,4 3 . Particle interactions will thus contribute
signi® cantly to heating and cooling rates and the effect of
solids fractions should be taken into consideration in
process design.
2.1.4. Particle rotation
The slip velocity between particle and ¯ uid will not be
due to translational ¯ ow alone, but will also result from any
particle rotation. An estimate of the possible enhancement
of heat transfer can be made by assuming that the rate of
rotation about the z axis, x , of food particles ¯ owing in a
pipe is approximately equal to the ¯ uid vorticity (as
suggested in experiments by Stockman4 4 ), i.e.,
1 ¶ufy ¶ufx
x = 2 ¶x - ¶y , (3)
where uf x and uf y are the ¯ uid velocities in the x and y
directions, respectively. For fully developed laminar ¯ ow
¶ufy / ¶x is zero, so the ¯ uid velocity distribution in the xy
plane is given by:
rt2
ufx = ufmax 1 - R2t
, (4)
where rt represents radial position within the tube, Rt is the
12 BARIGOU et al.
tube radius, and uf m a x is the maximum ¯ uid velocity on the
centreline. Combining equations (3) and (4) leads to:
r particle size on hf p will be due in part to the rise in the
x = - ufmax t2 , (5)
Rt
where the negative sign indicates that the rotation is
clockwise.
In food processing, a typical mixture in a tube of radius
0.05 m would have a maximum centreline velocity of about
0.1 ms- 1 . Therefore, the maximum particle angular velocity
(i.e. at rt = Rt ) will be 2 s- 1 . Using the expression derived
by Krieth et al.4 5 (equation (10)) the maximum Nusselt
number around a typical food particle (e.g. a carrot in
water), of diameter 10 mm, would be equal to 13.
The magnitude of this Nusselt number shows that particle
rotation can appreciably enhance particulate heat transfer.
However, the analysis of Stockman4 4 was for a single
particle ¯ owing in a tube. The observations of Lareo1 5 show
that, for solids concentrations above 5%, particles near the
tube wall where maximum rotational velocities are expected
to occur, appear not to rotate; due to the ¯ ow deformation
caused by high particle concentrations. This suggests that it
is not safe to assume heat transfer is enhanced by particle
rotation in food ¯ ows; more work is needed before the
effects can be con® dently incorporated in process design.
2.1.5. Particle size: wall-particle effects
Particle size is an important parameter which in¯ uences
hf p : as the particle-tube diameter ratio increases, the effect
of the wall will become increasingly important. Particle-
¯ uid heat transfer coef® cients have normally been measured
in a uniform ¯ ow ® eld: the velocity gradient near a wall will
result in distribution of relative velocity across the particle.
Con¯ icting results for the effect of this have been reported
in the literature. Sastry et al.4 6 , using a moving thermo-
couple attached to a metal sphere in water, obtained results
which showed an increasing hf p with increasing particle-
tube diameter ratio. More recently, however, Balasubrama-
niam and Sastry3 4 detected a much less signi® cant trend in
CMC solutions. The discrepancy between the ® ndings was
attributed to the difference in ¯ ow regimes studied
(turbulent for water, Re = 7300±43600; and laminar for
CMC, Re = 0.0058±798) and the associated effects of
particle radial location. Particle radial location was not
controlled in either study but would be expected to matter
more in laminar ¯ ow, where the velocity distribution is
highly non-uniform. This data is dif® cult to reconcile with
that of (i) Mwangi et al.3 5 who, working with freely moving
particles containing a melting point indicator, reported
considerable increases in hf p (58.3- 1301.3 Wm - 2 K- 1 ) with
increasing particle size (8.0±12.7 mm) in glycerine solu-
tions (Rep = 73.1-369.4) within a holding tube of 50.8 mm
dia.; and (ii) Kelly et al.2 7 who detected a decrease in hf p
with increasing particle size in open channel ¯ ow.
One problem with interpreting the data is the dif® culty in
determining relative velocities. This may explain observa-
tions such as those of Zuritz et al.2 8 who used three different
sizes (20.6±28.2 mm) of mushroom-shaped aluminium
particles in a CMC solution, and reported an increase in
hf p (548-700 Wm - 2 K- 1 ) with particle size. However,
Chandarana et al.2 6 using various sizes of diced carrot
particles and silicone cubes in water, found that hf p
decreased with increasing cube size. However, whilst
Zuritz et al.2 8 experimented on a narrow tube, Chandarana
et al.2 6 used a pipe of very large section. The in¯ uence of
relative velocity between ¯ uid and particle, due to a
reduction in the effective ¯ ow area in the presence of
larger particles.
2.2. Experimental Studies of Food Flows
The above discussion shows that the literature is contra-
dictory in places. The discrepancies and inconsistencies
could be due to experimental error, but it is more likely that
they result from the different experimental techniques used
and the dif® culty in de® ning and relating the experimental
conditions under which they were used. Research using
standardized experimental approaches is required to pro-
duce data from well-characterized situations.
It must be noted that in this paper data has been quoted as
reported in the original references. The accuracy of some of
the results is doubtful (too many signi® cant ® gures) given
the dif® culties associated with the experimental techniques.
Determination of the particle-¯ uid heat transfer coef® -
cient requires information on particle temperature history
under realistic conditions: correlating the data requires
information on the ¯ ow ® eld around the particles. The
dif® culty of monitoring, either directly or indirectly, the
temperature of a moving particle without interfering with its
motion, has led a number of investigators to resort to the use
of stationary particles in determining hf p (such as Chang and
ÊstroÈm and
Toledo3 3 ; Chandarana et al.4 7 , 6 9 ; Zuritz et al.2 8 ; A
48 36
Bark and Mankad et al. ). Because of the dif® culty in
measuring the temperature inside a food particle ¯ owing in
a continuous process, some food manufacturers also resort
to the use of ¯ uid-particle heat transfer simulation systems
which measure temperature transients inside a stationary
particle. For example, Dignan et al.4 9 cite a manufacturer of
aseptic processing equipment that offers such a simulation
system (the Continuous Process Simulator, Cherry-Burrell
Corp, Cedar Rapids, Iowa). In this type of simulator, the
particle is ® xed on the end of a temperature sensor, allowed
to equilibrate to a uniform initial temperature, and then
heated by a continuous hot stream of the product liquid
phase. The temperature transient is then used to calculate
the F-value for the product. In the test, care is taken to avoid
thermal channelling effects, i.e. allowing heat to travel
down the temperature probe to the centre of the particle. The
rate of heating will be a function of hf p , and thus the ¯ uid
velocity; any simulator must, therefore, allow accurate
measurement and control of this velocity.
The true relative velocity between particle and ¯ uid in the
real processing system must be used in the test. This is
dif® cult, both because particles will travel at different
velocities in a real system, and because the contribution of
particle rotational motion is not usually known. Conse-
quently, when applying the information gathered from a
simulation test to the design of a process, a conservative
approach, i.e. an unrealistically low hfp , is usually adopted.
Simulators with stationary particles can provide valuable
data that can be used to validate mathematical models or
check measurements from other experimental techniques;
however, the experimental set-up does not take into account
the particle dynamics of a real solid-liquid ¯ ow. A number
of different experimental approaches have been developed
Trans IChemE, Vol 76, Part C, March 1998
 HEAT TRANSFER IN TWO-PHASE SOLID-LIQUID FOOD FLOWS
for determining hfp between a moving particle and its carrier
¯ uid; these are discussed below.
2.2.1. Biological or biochemical methods
Biological or biochemical methods of assessing the
effectiveness of a continuous heat treatment process use
bacterial spores or biochemicals which are encapsulated
inside a carrier. The inoculated carrier is introduced in the
¯ ow, and after the heat treatment, the remaining concentra-
tion is determined. The principle has been exploited in
different ways to determine the heat transfer coef® cient,
albeit indirectly.
2.2.1.1. Particles inoculated with spores
The `biological thermocouple’ system has been used for
the last 30 years. Bacterial spores are used to monitor the
lethality of the process. These are encapsulated in a carrier,
so the spores do not come into direct contact with the food
product. Measurements are thus not affected by factors such
as pH, oxidation/reduction, and food nutrient level. By
measuring the number of surviving spores at the end of a
process, the sterilizing ef® ciency of a commercial heat
preservation food process can be determined.
This concept has been used successfully to measure the
lethality delivered to cans by P¯ ug and coworkers5 0 ± 5 6 ; here
the biological indicator units were rods of 2 in length and
0.25 in diameter. The technique has been extended to
continuous ¯ ows by Hersom and Shore5 7 , who used 5 mm
diameter glass bulbs, carrying a known number of spores,
inserted inside food particles to measure the heat treatment
delivered to the particle centres in a continuous system.
These type of units have a number of advantages: (i) the
location of the spores in the particle is precisely known, i.e.
they are located near the centre of the particle; (ii) when a
bulb is recovered it is clear that all the spores have been
recovered; (iii) the calibration procedure gives an accurate
experimental relationship between the number of surviving
spores and the F-value, thus obviating the need to measure
the exact inoculum level (N0 ) and thermal destruction rates
(D-values). When a large number of samples are assessed an
accurate estimate of the F-value delivered to the centre of
the particles can be obtained.
A related approach has been used for many years to assess
biologically the sterilization of retorted low-acid canned
food products. This involves inoculating the geometric
centre of a number of actual food particles with heat
resistant bacterial spores. It has been used in continuous
¯ ows; examples include Bacillus stearothermophilus in
calcium alginate particles2 5 , and PA3679 in turkey cubes5 8 .
The inoculated particles are recovered at the end of the
process, the number of surviving spores is evaluated through
a count-reduction procedure, and the sterilization of the heat
treatment is determined. In canning, the concept is simple
and can be implemented readily. It is much more dif® cult to
do in continuously ¯ owing systems, the major obstacles
being: (i) a large number of particles is required if the
process is to be reasonably assessed; (ii) the particles must
maintain their integrity throughout the system; (iii) ideally,
the inoculated particles should be recovered at exit from the
holding tube and instantly cooled to mimic the possible case
of a particle breaking up at the beginning of the cooling
phase. Some data for heat transfer coef® cients was obtained
by Heppell2 5 using this method. These results are probably
Trans IChemE, Vol 76, Part C, March 1998
13
not accurate, due to problems in getting an accurate count,
but it represents a very valuable attempt.
This method needs calibration data for the number of
viable spores in the food product as a function of F, against
which the actual measurements can be evaluated. These can
only be obtained through quantitative studies of spores
in the product. Dignan et al.4 9 have discussed the prob-
lems encountered in direct inoculation of food particles to
study continuous ¯ ows; the accuracy of the method depends
on a number of key factors including: (i) calibration must be
conducted under identical conditions of micro-organism
destruction as for the tests of the actual process; (ii) the
exact inoculum level for the particles (N0 ) must be
determined as some spores will leak out of the particles;
(iii) the residence times of the inoculated particles must be
representative of the fastest particle in the system; (iv) the
size of the spore carrier particles must be representative of
the largest particle size in the process, and they must
maintain their full size during the test programme. The
spatial distribution of the bacterial micro-organism within
the particles must also be known; if spores are distributed
throughout the particle the result will be an integrated
sterilization value rather than the sterilization value for the
slowest heating point.
2.2.1.2. Simulated food particles inoculated with bacterial
spores
The problems associated with the use of biologically
inoculated food particles to validate continuous sterilization
processes has led some researchers to use simulated
particles as biological indicators. For example, Hunter5 9
used Bacillus anthracis inside polymethyl-methacrylate
spheres. Spores in this material, however, are subjected to
dry heat destruction, so that the death rate becomes a
function of the moisture content of the plastic. Dallyn et al.6 0
who used inoculated alginate-gel particles found that spores
in alginate systems are stable for long periods of time and
yield reproducible results.
Most of the dif® culties associated with the use of
inoculated food particles are also present when using
simulated particles; the advantages of using simulated
particles being that particle size is uniform and controlled,
and the inoculum level can be uniform throughout the
particle. Such systems have been widely used by a number
of groups. Kim et al.6 1 ,6 2 describe the use of chemically and
microbiologically inoculated particles to examine the APV
ohmic heating process for sterilization of high-solids
fraction foods. They demonstrated the success of the
technique but did not attempt to obtain heat transfer
coef® cients, since, for validating an individual process, it
is necessary only to show that the design F-value is realized.
2.2.1.3. Time-temperature integrators
A time-temperature indicator (TTI) is a small device that
contains a microbiological or enzymic agent which will
undergo an irreversible time-temperature dependent change
when exposed to a heat treatment (for example Hendrickx
et al.6 3 ; van Loey et al.6 4 ). All TTIs require proper
calibration and testing under conditions representative of
the real process before experimentation2 2 . They are not
easily adaptable to real processing systems as extensive
experimentation is required to calibrate them under different
processing conditions.
14
Biological methods are simple in principle but rather
intricate in practice. They do not require transparent carriers
and can, therefore, be used under opaque ¯ ow conditions.
Successful implementation, however, requires a correct
technological approach, a well-controlled environment, and
accurate quantitative microbiology. These techniques can
be successfully used to prove that a process works,
but unless the whole temperature-time history of the particle
is recorded, they will not be suitable for measurements of
hf p .
2.2.2. Relative velocity method
In this method, the relative velocity between a transducer
particle and the carrier ¯ uid is measured from the
videotaped motion of ¯ uid tracers and the particle. The
technique has recently been employed by Balasubramaniam
and Sastry3 4 . Fine polystyrene particles (, 1 mm) were used
to trace the ¯ ow ® eld of CMC solutions (0.2, 0.5, 0.8%
conc) around a moving single aluminum particle (12.8, 16.0,
22.3 mm) in a glass tube (50.8 mm dia, 1.12 m length)
inclined upwards at 2.08%. The motion of the particle was
videotaped, and particle and tracer positions located using
square grids drawn over the tube. The slip velocity at
selected times was determined from the videotaped images
by following the passage of a selected tracer particle over
the test particle. Estimates of the surface heat transfer
coef® cient can then be obtained from standard correlations
available in the literature (see Table 1), such as:
Kramers 65 :
Nu = 2.0 + 1.3Pr0.15 + 0.66Pr0.31 Re0p.5 ,
5 ing the test liquid through a pump or by rotating the ¯ ask at
applicable over the range: Rep < 10 ; 0.7 < Pr < 400;
Ranz and Marshall66:
Nu = 2.0 + 0.6Re0p.5 Pr0.33 ,
4
applicable over the range: 1 < Rep < 10 ; 0.6 < Pr < 400;
Whitaker67 :
0.25
l
Nu = 2.0 + 0.4Re1/p 2 + 0.06Re2/p 3 Pr0.4
l p
applicable over the range: 3.5 ´ 104 < Rep < 7.6 ´ 104 ;
0.71 < Pr < 380; 1.0 < l / l p < 3.2.
where l and l p are the ¯ uid viscosities evaluated at the
mean bulk temperature, and at the particle-¯ uid interface
temperature, respectively. The limiting Nusselt number, for
thermal conduction at zero particle Reynolds number, can
be shown theoretically to be 2.0.
Balasubramaniam and Sastry34 found that, even though
the mean ¯ uid and particle velocities were similar,
signi® cant local slip velocities in the range 0.02±
0.19 ms- 1 were measured. Observation of the ¯ ow ® eld
around the particle also revealed the existence of the
following patterns: (a) translation, (b) rotation, (c) forma-
tion of vortices, and (d) particle tumbling in a radial
direction. Equations (6)±(8) were used to calculate hfp using
the measured slip values. The Ranz-Marshall correlation,
equation (7), yielded the lowest hfp values and the Whitaker
correlation, equation (8) yielded the highest. The results
showed hfp values considerably higher than those predicted
from zero slip velocity.
BARIGOU et al.
The following techniques rely on the direct determination
of the particle temperature history.
2.2.3 Thermocouple method
Here, a thermocouple embedded inside a transducer
particle records the temperature history at its centre. The
thermocouple method was ® rst used with stationary
particles (such as Zuritz et al.68; Chang and Toledo33 ;
Chandarana et al.69; Zuritz et al.28; A ÊstroÈm and Bark48 ;
Awuah et al. and Mankad et al. ). Zuritz et al.68 used a
70 36
static mushroom-shaped metal particle inside a tube through
which a non-Newtonian liquid was pumped at low rates.
Estimates of hfp in the range 548±1175 Wm - 2 K- 1 were
determined from temperature transients within the particle,
and the data were correlated in terms of Nusselt, Reynolds
and Prandtl numbers. These results, however, are not
representative of particle dynamicsunder real ¯ ow conditions.
To investigate the effects of the ¯ ow ® eld around a
particle, AÊstroÈm and Bark 48 immersed spherical/cubic (8±
17 mm) test particles of lead, polyacrylamide, calcium
alginate, and turnip inside a 200 mm diameter ¯ ask
containing 10 litres of either silicone oil or a 6% starch
solution. The temperature of the transducer particle and of
the ¯ uid 50 mm away from the particle was monitored.
From these measurements, hfp was determined (i) directly
from Newton’ s law of heating for particles for which
Bi < 0.1, or (ii) for particles with low thermal diffusivities,
by matching the theoretical solution of the heat conduction
equation with experiment using different hfp values.
Experiments were carried out with the ¯ uid at rest as well
(6) as in motion; ¯ uid motion was created either by recirculat-
different speeds with the particle position at different radii
in the liquid bath. The effects of the ¯ ow ® eld around the
particle, particle size and shape, particle and ¯ uid thermal
(7) properties, and ¯ uid viscosity were investigated.
Both natural and forced convective ¯ uid motion was
found to affect hfp strongly. The free convective ¯ ow due to
the introduction of a cold particle into a static liquid gave hfp
values in the initial phase of the temperature transient, 2 to 5
, (8) times higher than during the rest of the experiment. Heat
transfer coef® cients found from the middle and the end
periods of the transient were very similar indicating that the
effect of free convection became small. In contrast, when
liquid was circulated around the particle the maximum hfp
due to free convection was experienced at the end of the
heating curve. Initially, heat transfer between the cold
particle and the hot liquid is retarded by a cool interfacial
liquid layer of high viscosity, leading to a lower hfp . As the
particle heats, this surface layer heats, leading to the
magnitude of hfp being determined by the ability of the
surrounding ¯ uid to continuously supply the particle surface
with hot ¯ uid. When a lead sphere or cube was located at the
centre of the rotating vessel, i.e. exposed to ¯ uid in pure
rotation, hfp was similar to that obtained in stagnant liquid
(, 100 Wm - 2 K- 1 ). As the particle was moved 11 mm away
from the centre, where the ¯ ow ® eld could be described as
eccentric rotation, hfp increased in the range 100±
170 Wm- 2 K- 1 , as the rotational velocity was increased
from 0 to 60 rpm; at 60 rpm the slip velocity was
0.069 ms- 1 . At a position 50 mm from the centre, where
¯ uid motion is mainly translational, the ability to renew hot
¯ uid at the particle surface was considerably higher which
Trans IChemE, Vol 76, Part C, March 1998
 HEAT TRANSFER IN TWO-PHASE SOLID-LIQUID FOOD FLOWS
led to enhanced hfp values in the range 110±450 Wm- 2 K- 1 ,
as rotation increased from 0 to 60 rpm; at 60 rpm, the slip
velocity was 0.31 ms- 1 which is representative of ¯ uid ¯ ow
past a sedimented particle in a process plant.
Extensive static-particle experiments were conducted by
Mankad1 1 and Mankad et al.3 6 using a 15 mm static hollow
copper sphere to measure the ¯ uid-particle heat transfer
coef® cient. The sphere consisted of a thin copper shell
(0.5 mm) and contained a germanium resistance heater. Two
K-type thermocouples measured the surface temperature;
one at the front stagnation point, and one at 90 degrees to the
front stagnation point, with the aim of monitoring the sphere
surface temperature to detect any variations in heat transfer
coef® cient with radial position. The particle was used in a
¯ ow loop measuring 2.5 m in total length, and 0.1 m in
diameter; to ensure a smooth steady ¯ ow, a ¯ ow calming
section consisting of a bundle of narrow capillaries was used
upstream to give a ¯ at ¯ uid velocity pro® le. This simpli® es
estimation of the ¯ uid velocity at the particle face.
Experiments were conducted with water (Rep = 292±
2433), PAA (Rep = 114±893), and Glycerol solutions
(Rep = 5±140), over a ¯ uid temperature range 13- 188 C.
The solid surface temperature varied between 23- 358 C.
The work consisted of: single particle experiments where
the particle was positioned in the centre of the tube; two-
particle experiments where the heat transfer coef® cient of
the transducer particle was measured at varying distances
behind another similar particle in the tube to investigate
particle wake effects; packed bed experiments where the
heat transfer coef® cient was measured for a sphere in a close
packed arrangement of spheres; and variable voidage bed
experiments to simulate real continuously ¯ owing food
mixtures.
For a single isolated particle the results were in good
agreement with the predictions of the Ranz-Marshall
correlation (equation (7)). In the two-particle experiment
Nu values were only slightly enhanced (, 10%) when the
inter-particle distance was increased from 10 to 50 mm. This
enhancement was attributed to the reduction in boundary
layer thickness around the transducer particle; eddies
generated by the upstream particle, superimposed on the
¯ ow ® eld around the transducer, give mixing that reduces
the ¯ uid boundary layer thickness and thus resistance to heat
transfer. The Ranz-Marshall correlation was able to predict
hf p for the two-particle system, but only outside the laminar-
turbulent transitional ¯ ow regime (Rep < 500 6 250). When
the transducer particle was located within a randomly
packed bed of hollow polypropylene spheres of the same
diameter, the Nu values, for similar Rep values, were on
average 2.3 times higher than for an isolated particle. The
enhancement was small at low Re; satisfactory agreement
with the Ranz-Marshall correlation was obtained for Re less
than about 100. At high Re, eddy formation and recircula-
tion caused by adjacent particles may have been responsible
for the greater increase in heat transfer observed. Signi® cant
channelling can also occur in randomly packed beds where
there are large variations in local voidage, and may increase
or decrease local heat transfer rates. Channelling effects also
increase with tube Reynolds number. Experiments with
variable voidage beds involved locating the transducer
particle in the centre of a partially packed arrangement of
15 mm polypropylene spheres. The sphere spacing was
varied to give spatially uniform packing voidages of 70, 80,
Trans IChemE, Vol 76, Part C, March 1998
15
and 90%. Heat transfer to the particle was found to increase
with decreasing voidage. This increase was dependent on
the Reynolds numbers (tube or particle), with a high
dependence for water (high Re’ s) and a low dependence for
glycerol (low Re’ s). Again, for any bed voidage, the Ranz-
Marshall correlation was only found to be suitable at low
Reynolds numbers (, Re < 100).
The thermocouple method has also been used with moving
particles2 1 ,3 4 ,4 6 . The approach was introduced by Sastry et
al.2 1 ,4 6 ; a thermocouple was attached to a hollow aluminium
sphere (13.3±23.9 mm dia), with a wall thickness which gave
it a density similar to that of a food particle (1006 kgm- 3 ).
The design was chosen to allow Newton’ s law of heating
(equation (2)) to be used whilst also allowing a more realistic
simulation of the dynamics of a real food particle.
The temperature history of the particle was determined
whilst moving it in the ¯ uid with the same speed as that of
a free particle. In the studies of Sastry et al.2 1 ,4 6 , the
mean velocity of the particle without the thermocouple
attached was measured using two photoelectric sensors
located at either end of the ¯ ow section. When the
thermocouple was attached to the particle, the thermocouple
wire was pulled from the downstream end at the same
velocity as that of a free particle. The initial stage where the
particle undergoes an acceleration from zero velocity upon
introduction into the ¯ ow to the desired velocity was
omitted from the analysis, as the slip velocity during this
stage is very high and is not truly representative of real ¯ ow
conditions in holding tubes. Tests were conducted in ¯ ow
sections 0.4- 1.3 m long and for ¯ ows in the range 2.69-
6.68 ´ 10- 4 m3 s- 1 . The method was modi® ed by Balasu-
bramaniam and Sastry3 4 so that the transducer particle was
not pulled from the downstream end, but instead was
introduced from upstream. This reduced the time required to
match the velocity of the thermocouple-attached particle to
that of a free particle.
The stationary thermocouple method has the advantage of
being relatively simple and can be used with opaque ¯ uids.
However, the technique will underestimate hfp because the
¯ ow ® eld around the transducer particle is not fully
representative of the true ¯ ow ® eld surrounding a freely
moving particle. One interesting recent modi® cation is
Clement et al.7 1 who use a stationary particle in which a heat
pipe is inserted; the total heat ¯ ow to the particle can then be
measured. The ingenious moving thermocouple method as
used by Sastry and coworkers is more complicated than the
stationary particle method but allows the effects of ¯ ow to
be estimated. One problem is that the thermocouple wire is
likely to interfere with the particle dynamics and, in
particular, restrain its rotational motion: presumably the
method will still underestimate the true value. Neither
method gives the particle its total freedom: the next sections
consider possible alternatives in which the particle ¯ ows
freely through the tube.
2.2.4. Liquid crystal method
Stoforos and Merson7 2 , and subsequently Balasubrama-
niam and Sastry3 4 ,7 3 , and Zitoun and Sastry3 0 , have used a
method whereby a free moving particle is coated with a
liquid crystal. The liquid crystal, being heat sensitive,
changes colour gradually and reversibly with temperature as
a result of molecular structure rearrangement. The colour-
temperature response of the liquid crystal can be calibrated,
16 BARIGOU et al.
and the particle temperature history is inferred either from
visual colour determination, or (more accurately) from
image analysis of the videotaped colour changes. Balasu-
bramaniam and Sastry7 4 have reviewed the use of thermo-
chromic liquid crystals in heat transfer studies and their
applications to food processing research.
Stoforos and Merson7 2 used the method to measure hf p for
spherical particles in axially rotating cylinders. They
reported a value of 2326 Wm - 2 K- 1 for 25.4 mm Te¯ on
particles in water in a cylinder rotating at 102 rpm. Using
this technique, Balasubramaniam and Sastry3 4 measured
values of 857-2010 Wm - 2 K- 1 for particles in CMC
solutions in tube ¯ ow (see Table 1), and in scraped surface
heat exchangers7 3 . The same technique was employed by
Zitoun and Sastry3 0 to determine hfp values in the range 551±
887 Wm - 2 K- 1 for aluminium cubes in CMC under various
experimental conditions. Effects of ¯ owrate, viscosity,
particle size, and radial location were investigated.
Gadonna et al.7 5 have further developed the technique by
using a transducer particle made up of two concentric spheres,
the core of the particle was a polypropylene sphere precoated
with a black paint and then coated with a liquid-crystal; this
was subsequently coated with a layer of transparent epoxy
resin of known thermal diffusivity. The coating protects the
liquid crystal from the ¯ uid, frictional wear and ultraviolet
light; in addition, as the crystal is not in direct contact with the
¯ uid in the pipe, it changed colour progressively and much
more slowly, thus enabling easy detection of such colour
changes. Thermal equilibration of the test particle was
achieved in a thermo¯ ask before it was introduced in the
¯ ow. The procedure was based on visual determination of
changes in the liquid-crystal colour with temperature.
Tap water was pumped through a horizontal tube (3.10 m
length and 0.042 m dia) under the conditions: 1225 <
Re < 5434;0.216 < dp / dt < 0.571;1.016 < s < 1.050.Experi-
mentaldata for single particles were used with an inverse heat
conduction model to evaluate hfp . The results showed clearly
that particle ¯ ow behaviour, and in particular radial location,
slip velocity, and rotational motion had a predominant role in
determining hfp . Particle-tube diameter ratio was also found
to be an important parameter. Correlations for predicting hfp
under the various ¯ ow regimes investigated were proposed
(see Table 1).
The liquid crystal technique can provide useful informa-
tion, if properly used, but does have limitations. Colour
calibration is dif® cult; and it must be emphasized that each
calibration curve between temperature and Hue value is
unique as colour determination depends both on the
equipment and the environment in which it is used (different
lightening chambers, light bulbs, dust formation on light
bulbs, image processing system etc.). Furthermore, the
method can only be used with optically transparent liquids,
and cannot be used under UHT conditions since liquid
crystals cannot be used above about 1158 C.
2.2.5. Melting point indicator method
Mwangi et al.35 used an approach inspired by the liquid-
crystal method. A polymeric material that changes colour at
a speci® c temperature was located inside hollow transparent
particles, polymethyl-methacrylate spheres 8, 9.6, and
12.7 mm diameter. Colour indicators of different melting
points were placed inside the particles. Aqueous glycerine
solutions were used as the suspending ¯ uid. The time for the
surface of the indicator inside the particle to reach its
melting point and a colour change to be visually observed
was recorded. The particles containing the indicator could
not be reused as the colour change was irreversible.
Convective heat transfer coef® cients in the range 58.3±
1301.3 Wm- 2 K- 1 were obtained for nearly-neutrally buoy-
ant particles in shear ¯ ows inside a holding tube for particle
Reynolds numbers of 73.1±369.4. The heat transfer
coef® cients were found to increase signi® cantly with
increasing ¯ ow rate and particle-tube diameter ratio. Heat
transfer was enhanced by 80 to 200% when the particle
concentration was increased from a single particle to 3.22%.
Being a visual technique, the melting point indicator
method is limited to transparent ¯ uids and, therefore, can
only be used with model systems. Damay and Pain76 used a
similar phase change technique in which a particle is
introduced in a horizontal pipe and the change in its mass is
measured. The heat transfer coef® cient is then deduced from
a thermal balance on the particle equating the energy
supplied to the particle to the energy of phase change.
2.2.6. Remote temperature sensor method
All of the previous experimental techniques are limited
by the need to measure temperature either by thermocouple
or by an optical method. An ideal measurement technique
would be one in which the temperature of a particle could be
followed freely-moving non-invasively. Some progress has
been made with `temperature pills’ which use a particle with
a quartz crystal inside acting as the temperature sensing
element. The element resonates at a temperature-dependent
frequency and invokes a coil circuit and thus generates a
magnetic signal, as described by Balasubramaniam and
Sastry7 7 . An external receiver converts the magnetic signal
into a temperature reading. The temperature history of the
particle is monitored as it moves through the tube by
moving an external antenna along with the particle. The data
collected are then used in conjunction with a suitable
mathematical model to estimate hf p .
Bhamidipati and Singh3 1 ,7 8 were the ® rst to exploit this
technique. They used a cylindrical particle (22.6 mm length,
10.7 mm dia) of known density and speci® c heat capacity,
which broadcasts its temperature to an antenna coil, which is
moved along the outer surface of the tube as the particle
sensor moves inside the tube, allowing the temperature-time
pro® le of the particle to be obtained. The test ¯ uids were
aqueous CMC solutions (0.5±1.2% conc) heated to 82.228 C.
They reported hf p values for a single particle ranging from
108.08 to 195.83 Wm - 2 K- 1 .
Being non-invasive, the technique does not interfere
with particle trajectory as temperature is being measured,
and has the added advantage of yielding local hf p values.
However, the large size and density of the broadcasting
particle is severely limiting: it is crucial that the sensing
particle behaves the same way as the food. In addition,
quartz crystals used in the temperature sensor cannot
withstand high temperatures (>1218 C) which makes the
technique currently unsuitable for UHT processing. If the
particle were made smaller it would be a very attractive
technique.
A novel non-invasive technique is described by Ghiron
and Litch® eld7 9 who determine temperature using magnetic
resonance techniques: the change in temperature of a
magnetic particle is detected by its change in magnetization.
Trans IChemE, Vol 76, Part C, March 1998
 HEAT TRANSFER IN TWO-PHASE SOLID-LIQUID FOOD FLOWS
This type of technique offers the scope for real process
measurement, but is again not fully developed.
2.3. Experimental Studies in Process Engineering
Within process engineering the variation of Nusselt
number with particle-¯ uid relative velocity has been studied
by many workers over the last ® fty years, for single particle,
packed bed, and ¯ uidized systems. Few of the results are
relevant to heat transfer problems in food ¯ ows, but some of
the techniques used may be adapted to food applications.
The most fundamental work, and the basis of much
subsequent research, was that of Ranz and Marshall6 6 , who
examined evaporation of pure liquid drops (0.6 to 1.1 mm
dia) in air at 2208 C, for particle Reynolds numbers between
0 to 200, and developed the well-known Ranz-Marshall
correlation, equation (7).
Shallcross and Wood8 0 used published data to develop a
general correlation for heat transfer from spheres to air in
the particle Reynolds number range 100- 105 ,
Nu = 2 + 0.363Re0p.547 . (9)
These authors noted two important requirements in design-
ing experiments to determine heat transfer coef® cients
around a stationary particle: (i) the particle should be
supported at the rear stagnation point, and (ii) for laminar
¯ ow the inlet ¯ uid stream should have negligible turbu-
lence. The authors suggested that results from experiments
that do not observe these criteria can give Nusselt numbers
up to 10% too high. The use of cross¯ ow supports and
unsteady ¯ ow can thus lead to erroneous readings.
Particle rotation has been observed to occur within food
processing, particularly at low particle concentrations and
¯ owrates (for example by Liu et al.8 1 ). As discussed in
section 2.1.4, this rotational motion is expected to affect the
convective heat transfer coef® cient. Quantitative studies on
particle rotation in food ¯ ows are, however, very limited.
Some data is available in the general literature; for example
Krieth et al.4 5 studied the behaviour of rotating spheres in a
quiescent ¯ uid using 2 in and 6 in diameter metallic spheres
in water, air, oil, or mercury. Experiments were conducted
for Reynolds numbers based on angular velocity
(Rex = 2q f x R2p / l ) in the range 0 to 9 ´ 105 . The results
showed, as expected, that the convective heat transfer
coef® cient increased with increasing rotational velocity. It
was observed that at Reynolds numbers below 5 ´ 105 , a
¯ uid boundary layer separation zone was con® ned to 2
degrees either side of the equator (measured using
photographs); above this Reynolds number the separation
zone increased beyond 2 degrees, in proportion to the
angular velocity, thus enhancing the heat transfer. Situations
of interest to food processing usually involve low Reynolds
numbers of the order of 100 or less, since the carrier ¯ uid is
usually a viscous solution (e.g. sauce, syrup). Two
correlations were derived from these results; the low Re
limit is:
Nu = 0.43Re0x .5 Pr0.4 (10)
for Gr < 0.1Rex ; Rex < 5 ´ 10 ; 0.7 < Pr < 217.
2 5
The effect of particle concentration on heat transfer was
considered in detail by Agarwal4 0 who produced a
correlation for the change in heat transfer coef® cient due
Trans IChemE, Vol 76, Part C, March 1998
17
to the presence of other particles,
Nupb = e - 1.23Nusp , (11)
where Nusp is the Nusselt number for a single isolated
particle at the same super® cial ¯ uid velocity as the packed
or expanded bed of voidage e , and Nup b is the Nusselt
number for a particle in an expanded bed. This is an
attractively simple correlation which has been used by
Nixon et al.8 2 as the basis for correlating data for food-type
¯ uids and shown to work well: such an approach may be
useful for other workers.
3. OTHER FACTORS AFFECTING HEAT
TRANSFER
3.1. Wall-Fluid Heat Transfer
3.1.1. Estimations of wall-¯ uid heat transfer coef® cient in
food processing
The convective heat transfer coef® cient, hw , between the
¯ uid-particle mixture and the processing tube surface is not
well characterized in food processing, in particular with
respect to the effect of particle loading. This parameter is
crucial in determining the heating tube length, and hence
indirectly affects the holding tube length (as particulate
heating is related to ¯ uid heating rates/residence time).
Mathematical models (such as Mankad1 1 ) suggest that the
wall-¯ uid heat transfer coef® cient is as important for
process heat transfer as is the ¯ uid-particle heat transfer
coef® cient. Existing research in this area is sparse and there
are no sound studies on the effect of hw on sterilizer design.
This is re¯ ected in the wide variety of conventions used by
various authors who have compiled mathematical models
for sterilizers. The wall heat transfer coef® cient has
previously been estimated using equations for liquid
laminar ¯ ow assuming constant wall temperature4 7 , turbu-
lent ¯ ow using the Dittus-BoÈelter equation8 3 , or entered as
an arbitrary value depending on the type of heater/cooler;
for example, in their computational models, SkjoÈldebrand
and Ohlsson8 4 ,8 5 adopted a value of 1200 Wm - 2 K- 1 whilst
Mankad and Fryer3 8 used a value of 225 Wm - 2 K- 1 . For a
given system, these different approaches give widely
different estimates for hw . In addition, they are all based
on conservative design assumptions rather than hard
experimental data, and do not take into account particle
effects which are likely to be signi® cant. It is, therefore,
evident more data on wall-¯ uid heat transfer in food ¯ ows is
needed.
One recent study by Sannervik et al.1 2 determined wall
heat transfer coef® cients in a tubular heat exchanger
(35.6 mm dia, 6 m length) by measuring inlet and outlet
temperatures and performing a heat balance on the system.
The ¯ owing mixture consisted of sodium alginate particles
of average diameter 5.6 mm suspended in a 4% pseudo-
plastic starch solution. Particle concentrations of 0, 10, 20,
and 30% were used. Experiments showed that (i) the
presence of particles had a strong in¯ uence on heat transfer
rates from the wall, and (ii) wall heat transfer coef® cients in
the heating section were always higher than in the cooling
section because of lower liquid viscosity in the thermal
boundary layer. An increase in particle concentration from 0
to 10% approximately doubled hw in both sections.
Increasing the solids loading from 10 to 20% and from 20
18 BARIGOU et al.
to 30% led to further heat transfer enhancements of , 25%
in the heating section and , 35% in the cooling section.
A plausible explanation is that particles interact with the
wall boundary layer, causing ¯ uid mixing and enthalpy
exchange with the ¯ uid inside the pipe, a mechanism similar
to heat transfer by turbulent eddy convection. The authors
suggested the use of an equation originally proposed by
Singh8 6 for a single-phase power-law ¯ uid with a fully
developed velocity pro® le:
3n + 1 1/ 3
Nu = 1.75 Gzm , (12)
4n
where n is the power law index, Gz = MCp /kl is the Graetz
number (M is mass ¯ ow rate, l is heater/cooler length, k is
thermal conductivity,and Cp is speci® c heat capacity). For a
single phase liquid the equation has a theoretically derived
exponent m = 1/3. For solid-liquid mixtures, Sannervik et
al.1 2 found that overall m increased with particle concentra-
tion in the range 0.297-0.519, and had slightly higher values
in the cooling section than in the heating section.
One reason for this lack of progress has been the lack of
adequate techniques for measuring heat ¯ ow across a pipe
wall to a two-phase mixture. Heat ¯ ux sensors may provide
an attractive solution to this problem. These have been used
in a wide range of applications such as determining the
thermal properties of insulation systems, heat loss determi-
nation in building structures, monitoring solar heat collector
performance, and aerodynamic wind tunnel studies (see
for example, Ortolano and Hines8 7 and Mohan et al.8 8 ). The
food industry, however, does not seem to have exploited
such transducers, which consist of a differential thermo-
couple with a thin foil type thermopile bonded to both sides
of a known thermal barrier; the difference in temperature
across the thermal barrier is proportional to the heat ¯ ow
through the sensor, which is attached to the surface of the
pipe. Nixon et al.8 2 have shown the feasibility of the
technique.
3.1.2. Estimations of wall-¯ uid heat transfer coef® cient in
process engineering
Heat transfer between a surface and a ¯ uid is ubiquitous
within process engineering through the study of heat
exchangers. A considerable volume of literature exists on
the prediction of heat transfer; however, the majority of this
literature is not relevant to estimating the wall heat transfer
coef® cient in food ¯ ow, because the packed and ¯ uid bed
heat transfer literature is largely concerned with gas-solid
systems.
SchluÈnder8 9 reviewed transport processes in packed beds,
and highlighted that void fractions can be greater at the wall
than in the bulk. For a randomly packed bed of uniform
spheres the bulk voidage is about 0.4, whilst the wall
voidage can reach 0.5. A two channel model, representing
¯ ow at the wall and in the bulk, was developed to evaluate
the velocity ratio between ¯ uid at the wall and ¯ uid in the
bulk, using the Ergun equation,
D P 150l uf (1 - e ) 1.75q f u2f (1 - e )
2
l = e 3 dp2
+ e 3 dp
, (13)
where l is the length of the bed and D P is the pressure drop
through the bed, to obtain expressions for the ¯ uid velocity
in each channel, which were then combined to give an
equation for the velocity ratio. For a randomly packed bed
of spheres, it was shown that the velocity of the ¯ uid at the
wall was 2.81 times greater than that of the ¯ uid in the bulk
of the bed. This shows that where variations in cross-
sectional voidage occur, appreciable ¯ uid bypassing can
arise. In a food ¯ ow, this might give signi® cant channelling
around localized zones of high solids concentration leading
to variations in particle heat transfer coef® cients within
the ¯ ow. Furthermore, high ¯ uid velocities near the wall
would invalidate the often-used assumptions of fully
developed laminar or turbulent ¯ ow in estimating the wall
heat transfer coef® cient. Experimental work on packed beds
has con® rmed that the presence of particles in a tube may
result in ¯ ow channelling at the wall4 1 . This can lead to
signi® cantly higher heat transfer coef® cients than those
occurring in a tube conveying a single phase ¯ uid. This
work is important in providing insight into particle effects
on heat transfer taking place at the wall.
Gunn and Khalid9 0 investigated wall heat transfer
coef® cients in packed beds, using an externally heated
packed bed (diameter 3.75 in, length 12 in), ® lled with either
lead shot, glass ballotini, or nickel particles, in the range
1- 7 mm. Compressed air was passed through the bed and
the particle Reynolds number varied between 1 and 400.
The air temperature was measured at the entrance of the bed
and over the cross section of the exit by means of several
annular banks of thermocouples. This information was used
together with the ¯ uid ¯ owrate and wall temperature to
estimate the wall heat transfer coef® cient. The wall Nusselt
number was found to vary linearly with particle Reynolds
number, the values ranging between 1.5 and 150; no
correlation could be derived due to the high amount of
scatter in the results.
Dixon et al.9 1 determined the diffusive mass transfer
coef® cient between the inner surface of a tube coated with
a thin layer of water soluble material (2-naphthol,
cinnamic acid, or benzoic acid) and a packed bed of
large particles. Water was pumped through the packed
column to allow the soluble material to dissolve from the
walls, and the exit ¯ uid stream was sampled at different
radial positions for solute content. Different particle
diameters were used so that the tube to particle diameter
ratio varied between 3 and 12 (in food processes this ratio
typically falls between 4 and 8); the particle Reynolds
number was in the range 50-500. Differential mass balances
were used to estimate the wall mass transfer coef® cient, and
data were correlated by
1.5
dp
Shw = 1.0 - 1.5
dt
Sc1/ 3 Re0p.59, (14)
where Shw is the wall Sherwood number and Sc is the
Schmidt number.
In a more recent paper, Jamialahmadi et al.9 2 measured
heat transfer coef® cients to a solid-liquid ¯ uidized bed in a
cylindrical tube (D = 23.8 mm; l = 160 mm) with water as
liquid phase and cylindrical steel particles (dp (mm) ´ l
(mm) = 1.0 ´ 1.0; 1.6 ´ 1.6; 2.5 ´ 2.5), glass (2, 4.5 mm dia),
nickel (4.5 mm dia), copper (4.5 mm dia) and lead (4.5 mm
dia) spheres as solid phase. The suspended solids gave rise
to enhanced heat transfer, but no further improvement was
observed once the behaviour of the bed changed from
Trans IChemE, Vol 76, Part C, March 1998
 HEAT TRANSFER IN TWO-PHASE SOLID-LIQUID FOOD FLOWS
particulate to aggregate. The results were modelled using
analogy with nucleate-boiling heat transfer; this predicted
the experimental results together with extensive data from
the literature with good accuracy. The work resulted in the
following correlations:
for particulate ¯ uidization,
0.256
dp
hw = hc + 1.5 D
(1 - e )0.5075 hp - hc );
and for aggregated ¯ uidization,
dp 0.358
hw = hc + 8.64
D
(1 - e SB )
0.353
(1 - e )1.077 (hp - hc );
where, dp is particle diameter, D is ¯ uidized bed diameter,
hw is the wall heat transfer coef® cient, hc and hp are
convective heat transfer coef® cients for regions of the wall
unaffected and affected by particles (correlation data for
these coef® cients are given in the paper), e is ¯ uidized bed
voidage, and e S B is packed bed voidage. The correlations
were each compared to twenty six of the most frequently
recommended correlations in the literature, and were found
to have much smaller average relative errors of prediction.
The data suggests dependence on both particle size and
solids fraction; although it is not known whether any of this
type of correlation applies in foods, the data suggests ways
of treating food ¯ ow information. No set of results is
directly applicable to food ¯ ow situations where the solids
are entirely mobile; research is still needed to quantify the
wall heat transfer coef® cient in such continuous processes.
3.2. Mixing of the Liquid Phase
This review has shown that, of the data required for
design, most information is available on ¯ uid-particle heat
transfer and little is available on wall-¯ uid heat transfer.
However, the temperature distribution within the liquid will
also be very important: for example, it is possible that, for a
high viscosity carrier ¯ uid in which little mixing takes
place, transport of heat through the ¯ uid may be controlled
essentially by thermal conduction. It is commonly assumed
the liquid is stirred suf® ciently well that radial temperature
gradients can be neglected (see section 4); but there is very
little data available on the actual temperature gradients
within real food systems. Lefebvre and Leuliet9 3 show the
thermal ® eld within viscous liquids and show that very large
temperature gradients can arise in high viscosity solutions:
the controlling parameter is the ratio of the Grashof and
Reynolds numbers. High viscosity ¯ uids are commonly
used to minimize particle sedimentation; however, if they
result in low heat transfer rates product quality might be
lowered.
4. HEAT TRANSFER MODELLING
4.1. Modelling Studies in Food Processing
Ideally, to ensure the commercial sterility of continuously
processed solid-liquid foods without too much loss in
quality, thermal process calculations should be based on
accurate temperature-time data taken within particles as
they ¯ ow through the heating, holding and cooling sections
Trans IChemE, Vol 76, Part C, March 1998
19
of the sterilizer. However, as discussed above it is not
possible at present to measure the temperature of food
particles in continuous sterilizers. Mathematical techniques
using accurate experimental data (i.e. derived from systems
analogous to those occurring in industrial food processes)
are needed to estimate the temperature-time history in the
particle and hence ensure the correct level of sterility is
attained within the product without compromising its
(15a) quality.
A number of different modelling studies have been
carried out in an attempt to predict the temperature
variations within a particle moving through a continuous
aseptic process. Most of the models proposed to date
incorporate two fundamental assumptions: (i) there is zero
(15b) slip velocity between liquid and particle, hence it is often
assumed that Nu = 2 for particle-liquid heat transfer, i.e. that
the mode of heat transfer from liquid to particle is purely
conductive8 3 ; and (ii) the ¯ uid phase is a radially-mixed
plug ¯ ow with zero axial dispersion, in which all the
particulates travel at the same velocity4 7 . As noted already,
neither of these approximations is likely to be correct. The
section below describes how this problem has been
modelled; a model needs to re¯ ect experimental data to
predict ¯ uid and particle temperature pro® les across the
heating, holding and cooling sections.
4.1.1. Thermal balances
The simplest modelling technique is to carry out energy
balances for ¯ uid and particles in each section of the
process. This leads to the estimation ® rst of the particle
surface temperature, and then to the calculation of the
particle centre temperature. Once temperature pro® les at the
coldest points, usually the geometric centres of the particles,
are known, lethality and cooking levels can be calculated
using the standard equations (16a) and (16b), respectively,
t
F = 10(T - Tfref )/ zf dt, (16a)
0
where, F which is the F-value, is an equivalent heating time
for which the product could be held at a constant reference
temperature, Tf re f , to give the same ® nal concentration of
microbial pathogens as a processing time, t, for which the
temperature, T, changes. Tfr e f depends on the organism
being inactivated or the indicator organism used (e.g.
121.18 C for C. Botulinum), and zf is the temperature change
which produces a 10-fold change in reaction rate from
the rate at the reference temperature (e.g. 108 C for C.
Botulinum)1 ,2 .
Product quality loss is estimated using the cook value, C,
also known as the C-value, a parameter de® ned in a similar
way to the F-value, which gives a measure of the extent of
nutrient loss in units of time,
t
C = 10(T - Tcref )/ zc dt , (16b)
0
where Tc r e f is a reference temperature dependant on the
nutrient under consideration (typically 1008 C), and zc is the
temperature change which produces a 10-fold change in
reaction rate from the rate at the reference temperature
(typically 258 C)1 ,2 .
20 BARIGOU et al.
Models are required to calculate temperature pro® les;
those for calculating processing duties for a two-phase
mixture generally ® rst consider an energy balance on the
¯ uid over some incremental heat exchanger length8 3 ,
Outlet enthalpy of liquid =
inlet enthalpy of liquid + heat transfer from walls
+ heat transfer from particles
(Cp w)f (Tf + D Tf ) = (Cp w)f Tf + Uhx Ahx (Th - Tf )
+ hfpAp np (Tps - Tf ), (17)
where, Cp is speci® c heat capacity, w is the ¯ uid mass
¯ owrate, Tf is the ¯ uid temperature, Th the heat exchanger
wall temperature, Tp s the particle surface temperature, np is
the number of particles present in the section, each having
individual surface area Ap , Uh x is the overall heat transfer
coef® cient at the heating/cooling surface, and Ah x is the
heater/cooler surface area available for heat transfer. This
equation assumes radially uniform ¯ uid temperature.
The thermal response of the particle can then be predicted
by solving the transient heat conduction equation,
¶Tp
= .(kp = Tp ) = (Cp q )p . (18a)
¶t
The two phase thermal balances are coupled by the interfacial
convective heat transfer term between ¯ uid and particle,
= .(kp = Tp ) = hfp (Tf - Tps ). (18b)
These energy balances can be used in all sections of the ¯ ow
system. If the holding tube is adiabatic then the term
Uhx Ahx (Th - Tf ) in equation (17) can be neglected. Once the
temperature pro® les for the two phases are known, i.e. by
solving equations (17)±(18), then the level of sterility and
quality loss can be estimated from equations (16).
Many workers have adopted the above techniques to
analyse the sterilization process. The major dif® culties in
this approach are that (i) radial uniformity is assumed, and
(ii) in order to solve the above set of equations, the two
convective heat transfer coef® cients, hf p and hw , are
required. A too high or too low estimate can result in
either quality loss or an insuf® ciently sterile product.
4.1.2. Analytical solutions to the heat conduction equation
In a few idealized cases the solution to the heat transfer
equation is algebraic; many such solutions are given in texts
such as Carslaw and Jaeger 9 4 . For a sphere, equation (18a)
can be rewritten in spherical co-ordinates;
¶Tp a s ¶ r2 ¶Tp
=
¶t R2p ¶rp
p
¶rp
, (19)
and series solutions to equation (19) can be used if (i) the
particle is heated or cooled by contact with a constant
temperature environment, and (ii) the physical properties
are constant. Equation (20) shows the thermal response of a
sphere as a function of its radius, Rp , and time, t, expressed
in terms of the Fourier number (Fo = a s t/R2p ) when a sphere,
initially at Ti , is brought in contact with a ¯ uid at Tf
with in® nite heat transfer coef® cient at the ¯ uid particle
interface,
Tp - Tf ¥ sin(jp rp / Rp ) (-j2 p
=
2
2(-1)j+ 1 e Fo)
. (20)
Ti - Tf j=1
jp rp
Most of the early work on solids sterilization used this type
of equation, ® rst for canned foods, and then for particles in
continuous processing. One of the ® rst models was that of
Ball around 1920, developed by Ball and Olson9 5 for
sterilization during canning. At high t, all but the j = 1
solution of equation (20) (or its equivalent for other particle
geometries) are negligible, so the temperature transient
becomes a single exponential, and a semi-logarithmic plot
of temperature against time is linear. The difference in
temperature between the two phases at any instant is known
as the thermal lag; in the exponential region, this lag is
constant. Some modi® cations are needed to approximate the
non-logarithmic behaviour at the start and end of the
sterilisation process. Ball and Olsen9 5 derived an equation
for the accumulation of sterility in a process of heating
temperature, Th , and cooling temperature, Tc . The equations
are not fully accurate, but were put to effective use before
computers were available to solve equation (18a). They give
adequate results for heating but poor results for the cooling
stage.
More recently, Dail 9 6 modi® ed Balls method to calculate
holding times for different particle shapes. Series analytical
solutions for heat transfer into an in® nite slab and in® nite
cylinder were obtained to give equations similar to equation
(20) which were then simpli® ed, using only the ® rst terms of
the series. This was developed further by Larkin9 7 who
adapted the method to calculate holding times for food
processing systems where the semi-logarithmic tempera-
ture-time pro® le is not linear (i.e. the thermal response is not
purely exponential). This method uses a ® nite difference
solution of equation (18a) to calculate the centre tempera-
ture of a conduction-heated spherical particle moving
through the heat-hold-cool sections of an aseptic processing
system. The method was only approximate; it assumes both
that the heat transfer coef® cient is in® nite and that the ¯ uid
temperature pro® le is known.
4.1.3. Computational models
More rigorous models for continuous aseptic processing
have been developed in recent years, based on solid and
liquid energy balances, such as equations (17)±(18).
Formulation of the models requires assumptions about
heat transfer and ¯ ow behaviour, and the degree of
complexity of the constitutive equations depends on the
simplifying assumptions made.
Initial work did not attempt to solve the temperature
balance for the ¯ uid as well as the solid. de Ruyter and
Brunet8 assumed a linear ¯ uid temperature pro® le with time
through each component of the sterilizer. Using these preset
¯ uid temperatures the temperature of the solid phase was
calculated at each point in the sterilizer. The model was
used to estimate holding times for solids of different
diameters; as expected, longer holding times were necessary
to sterilize large particles compared to small ones. The
authors assumed that the convective heat transfer coef® cient
between solid and liquid was in® nite, and that both phases
moved at identical velocities through the system. The
assumption that the ¯ uid temperature pro® le is ® xed implies
Trans IChemE, Vol 76, Part C, March 1998
 HEAT TRANSFER IN TWO-PHASE SOLID-LIQUID FOOD FLOWS
that solids heating has a negligible effect on ¯ uid
temperature. Strictly, this assumption violates the law of
conservation of energy and in some cases can lead to serious
inaccuracies; for example, in the presence of a high
concentration of large particles, the effect of the solids
heat capacity would alter the ¯ uid temperature pro® le
signi® cantly. In such a situation, the supposition of a ® xed
¯ uid temperature pro® le becomes questionable.
Similar work was carried out by Manson and Cullen9 who
investigated the effects of particle residence times on the
overall lethality level of cylindrical solids moving through a
heat-hold-cool sterilizer. The model also used a ® xed ¯ uid
temperature pro® le, and solids temperatures were calculated
from these preset ¯ uid temperatures through the sterilizer.
The ¯ uid-particle interfacial heat transfer coef® cient was
assumed in® nite. This model represents the ® rst attempt to
consider residence time distributions. The holding tube was
modelled as eleven radial shells. Equal particle concentra-
tions were assigned to each shell, and the particle velocity
was then set equal to the maximum ¯ uid velocity, based on
fully developed laminar ¯ ow in the shell. This enabled a
range of particle velocities to be assigned, thus incorporating
the effects of a residence time distribution. No modi® cations
were made to the mass balance to account for differences in
solids velocity.
The results showed that a parabolic ¯ ow gave longer
heating and holding tube lengths than a plug ¯ ow particle
residence time distribution. Thus, assuming that all particles
remain in the system for equal times could result in
insuf® cient solids sterilization. No experimental validation of
the assumptions was given, but the model was a signi® cant
theoretical advance. Although it is questionablewhether solid
particles would adopt a parabolic velocity pro® le akin to that
of the ¯ uid6 , however, the ideas represented in the model are
clearly correct.
The ® rst model to calculate the liquid temperature pro® le
as well as the solid was that of Sastry8 3 who modelled
process schedules for mushroom-shaped particles of various
sizes at a constant concentration of 44%. The three stages of
the continuous aseptic process were modelled using energy
balances for each stage. Instead of modelling the effect of
particle size distribution, heat transfer to a group of average-
sized particles was evaluated. The ¯ uid-particle heat
transfer coef® cient was based on the limiting value for a
sphere in a stagnant ¯ uid, i.e. Nu = 2 which is the case for
zero slip velocity. The energy balances for the two phases
(equations (17) and (18a)) were solved simultaneously using
an iterative procedure. The ¯ uid temperature predictions
were then used as a time-dependant convective boundary
condition at the particle surface; this data was used to
determine particle temperatures.
Thermal balance equations were ® rst solved to establish a
¯ uid temperature pro® le along the tube, assuming particles
and ¯ uid travelled at the same velocity. The effect of this
liquid temperature pro® le on different particles and process
conditions was then studied. The ¯ uid temperature was set,
and the thermal response of the particle calculated
accordingly; no account was taken of any effect that the
particle had on the liquid temperature. This could cause
errors; for example when a large cold particle is heated by
the liquid, the liquid temperature will be reduced. Data on
the effect of velocity and particle size must, therefore, be
treated with caution. Subsequent simulations studied the
Trans IChemE, Vol 76, Part C, March 1998
21
effects of both particle size, and the two convective heat
transfer coef® cients (¯ uid-particle and wall-¯ uid). Data
were also presented for the processing of particles which
travelled at different speeds or which were of different sizes
to the uniformly sized particles used to establish the base
case.
The simulations showed that (i) the length of the holding
tube was sensitive to the heat transfer coef® cient only for
Bi <10, when external heat transfer is signi® cant2 0 ; (ii) as
the heat transfer coef® cient increased, the holding tube
length decreased to an asymptotic value corresponding to
internal-conduction-controlled heat transfer (i.e. Bi >10);
and (iii) the holding tube length decreased with increasing
average particle residence time, and increased with particle
size.
An investigation into different possible methods of
licensing sterilization procedures was carried out by
Chandarana et al.4 7 and Chandarana and Gavin9 8 for the
NFPA (National Food Processors Association) in Washing-
ton. When a product is licensed in the USA, it must be
shown to be sterile using an approved technique. A
mathematical model using three-dimensional transient
heat conduction equations and energy balances was
formulated to estimate heat transfer into foods passing
through a heat-hold-cool system. The model consisted of the
solution of: (i) equation (18a) for a cube, (ii) equation (17)
for the three cases of heating, holding and cooling using
different temperatures and heat transfer coef® cients which
were computed from literature correlations, and (iii)
coupling of the two phase thermal balances via solution of
equation (18b).
Three possible approaches to scheduling and licensing
commercial processes were considered, based on various
conservative assumptions:
(i) particles increase in both temperature and sterility in the
heat exchanger and holding tube;
(ii) increase in particle temperature occurs solely in the
holding tube, i.e. only the liquid is heated in the heating
section, and no sterility accumulates in the heating section;
(iii) both phases increase in temperature in the heat
exchanger, but sterility is assumed to accumulate only in
the holding tube.
Heat transfer between the particles and ¯ uid was
estimated for the conservative case of pure thermal
conduction between the solids and ¯ uid i.e. Nu = 2. The
integrated lethality of the particulate product was calculated
and the three models compared. Unsurprisingly, it was
found that case (i) was closest to an actual system, where
both temperature and lethality accumulate in both heater
and holding tube; this produced the most realistic results
(i.e. most similar to the results from an actual steriliser).
This work has formed the basis of the mathematical model
used to validate an aseptic process1 1 8 .
The model of Chandarana and Gavin9 8 was adopted by
Lee et al.9 9 to examine the in¯ uence of changes in input
parameters (i.e. product and process variables) on the
holding tube length required for sterility, peroxidase
retention and thiamine retention, the latter two related to
product quality and cook value. The study aimed to provide
insight into the possible margins of error in model
predictions due to inaccurate estimation of the input
parameters, such as particle and ¯ uid physical properties.
22 BARIGOU et al.
A summary of the main variables considered, and their
associated sensitivities is presented in Table 2. Over the
ranges investigated, particle size, particle density, particle
speci® c heat capacity, and product ¯ owrate had the greatest
effect on holding tube length and thiamine retention;
changes in peroxidase retention were minimal for all
parameters considered. The most sensitive factors in
determining the process were particle size and product
¯ owrate. Changes in ¯ uid properties such as thermal
conductivity and viscosity showed little effect on holding
tube length or cook value parameters. The study did not
consider parameters such as heat transfer coef® cients; the
effects of these may be more important than those examined.
McKenna and Tucker1 0 0 used a ® nite difference model to
predict the centre temperatures of cylindrical, spherical, and
cubic particles subjected to a constant ¯ uid temperature of
1358 C. The computed temperature history pro® les were then
used to estimate the F-value and C-value for the processed
product. The code was validated by comparing the
computed temperature-time pro® les with the pro® les
determined experimentally from a single transducer particle
with a thermocouple at its centre, placed in a ¯ ow loop
where the ¯ uid heated the particle; theory and experiment
were in good agreement. The convective heat transfer
coef® cient was an input variable in the model, and was
estimated using the Ranz-Marshall correlation (equation
(7)).
The model of SkjoÈldebrand and Ohlsson8 4 ,8 5 extends that
of Sastry8 3 by allowing a greater parameter variation to be
imposed on the sterilizer design. The liquid energy balance
was as used in the original model, but the solids energy
balance equations were modi® ed to allow calculations for
spheres or cylinders. The programme describes a system
comprising a chosen number of heating units, a holding
section, and a chosen number of cooling units. The product
¯ ows through the process at a selected mass ¯ owrate.
Conduction heat transfer is assumed within the particles,
although a convective boundary condition at the particle
surface is used to determine the rate of thermal interchange
with the ¯ uid. Other assumptions made are identical to those
in other models, namely that the liquid is perfectly mixed in
all sections of the sterilizer, that each particle is totally
surrounded by liquid, and that all particles have the same
size and geometry.
The model calculated processing duties, equipment sizes,
and product sterilization and quality measures. In each case,
all particles were considered spherical. Particle residence
times were simulated by inputting a ® nite value for the
Table 2. Sensitivity parameters; results of Lee et al.99 .
% change
Parameter in parameter
Particle size - 50% to + 50%
Particle loading - 50% to + 50%
Particle thermal conductivity - 10% to + 10%
Particle density - 2% to + 2%
Particle speci® c heat capacity - 2% to + 2%
Fluid thermal conductivity - 6% to + 6%
Fluid viscosity - 70% to + 70%
Product ¯ owrate - 25% to + 25%
velocity ratio of an average moving particle to the fastest
moving particle. Both phases were assumed to move at
identical velocities, hence heat transfer enhancements due
to slip were ignored. The heat transfer coef® cient between
the ¯ uid and the heater/cooler tube walls was arbitrarily set
at 1200 Wm - 2 K- 1 . The effects of various parameters on the
holding tube length were studied as follows:
(i) Particle-¯ uid heat transfer coef® cientÐ the holding tube
length generally decreased with increasing heat transfer
coef® cient, as shown by Sastry8 3 . At low heat transfer
coef® cients (<100Wm - 2 K- 1 ), the tube length was highly
sensitive to even small changes in hf p because of the low
particle Biot number. At higher values (>200Wm - 2 K- 1 )
even a large change in hfp had little impact on the length of
the holding tube.
(ii) Particle diameterÐ for small particles the desired
sterility was achieved in the heating unit; hence no holding
tube was required. Above some diameter, a function of the
sterilization temperature, thermal conduction within the
particle became an important factor in reaching the desired
sterilization temperature and thus in¯ uenced the holding
tube length required to achieve the desired level of sterility.
Above this critical diameter, further increases in particle
diameter generated a linear increase in holding tube length.
(iii) Particle concentrationÐ particle loading emerged as a
key factor in determining the holding tube length in that it
affected the heat capacity of the system; higher concentra-
tions required longer holding tubes. For the cases studied,
the ¯ uid had a greater thermal capacity than the solids.
(iv) Flow conditions in the holding tubeÐ the simulation
investigated the effects of varying the ratio of the average
liquid velocity to that of the fastest particle in the range 0.1±
1. A slow, approximately linear decrease was observed in
the holding tube length as the velocity ratio was increased.
It is not clear how the liquid temperature pro® le was
calculated for the cases where different conditions (such as
particle diameter) were simulated; it is not, therefore,
possible to tell whether this model represents a signi® cant
improvement on that of Sastry8 3 .
A recent model by Cacace et al.1 0 1 simulated particle
heating and holding for a 20% delivered solids concentra-
tion of 10 mm potato cubes in a sodium chloride solution,
using a ® xed ¯ uid temperature pro® le recorded from an
existing sterilizer and entered into the model as an input
variable. The particle temperature pro® le was estimated by
solving equation (18a) using the ¯ uid temperature as a
boundary condition. The value of hf p was assumed to be
% change in % change in % change in
hold tube length peroxidase retention thiamine retention
- 79% to + 142% + 4% to - 6% + 209% to - 90%
+ 10% to - 7% no change + 10% to - 8%
+ 10% to - 8% - 0.5% to + 0.5% - 15% to + 13%
- 4% to + 4% + 0.1% to - 0.1% + 4% to - 4%
- 3% to + 3% + 0.1% to - 0.1% + 3.5% to - 3.5%
+ 1.5% to - 1.5% no change - 1% to + 1%
- 10% to + 8% no change - 10% to + 8%
- 87% to + 208% - 1.2% to + 1.8% + 10% to - 75%
Trans IChemE, Vol 76, Part C, March 1998
 HEAT TRANSFER IN TWO-PHASE SOLID-LIQUID FOOD FLOWS
1000 Wm - 2 K- 1 . The code calculated the degree of
microbial spore destruction (Saccharomyces Cerevisiae)
for a particle cube as it moved through a heating/holding
arrangement. Unlike other models reported in the literature,
this was experimentally validated. The number of microbial
spores of Saccharomyces Cerevisiae was determined before
and after processing, and the results were compared to those
generated by the model; the theoretical and empirical results
were found to be in good agreement.
Additional experimental work was conducted to estimate
hf p by holding a potato cube stationary in a stream of ¯ uid
and recording the temperatures of the ¯ uid, particle surface,
and particle centre. The heat transfer coef® cient was then
related to slip velocity, although no correlation was derived.
The measured values of heat transfer coef® cient ranged
between 300 Wm - 2 K- 1 and 2000 Wm - 2 K- 1 for slip
velocities between 20 cms- 1 and 29 cms- 1 , respectively.
The average particle and ¯ uid velocities in the two phase
mixture were measured, and the slip velocities for this case
ranged between 0 and 5 cms- 1 ; these are signi® cantly higher
slips than those observed by Lareo1 5 .
Mankad et al.3 7 proposed a one-dimensional model to
study the effect of particle-liquid slip on a homogeneous
food ¯ ow, in which sterilizer lengths for various solid-liquid
slip velocities and delivered solids concentration were
computed at a ® xed ¯ ow rate. For low slip velocities, the
enhancement of interfacial heat transfer coef® cient reduced
the process length. The model was subsequently extended
by Mankad and Fryer3 8 to include non-homogeneous
strati® ed ¯ ows which can occur both in horizontal and
vertical situations6 . The model was used to study phase and
slip velocity effects that a heterogeneous ¯ ow might have in
a practical situation, and to demonstrate how a full model
might be used if ¯ ow patterns and particle residence time
distribution were known. The strati® ed ¯ ow was assumed to
consist of two interconnected one-dimensional ¯ ow zones.
A sedimented bed lying underneath a low particle
concentration region was modelled; (each with its own
solids fraction, phase velocities, and particle-liquid slip).
Slip velocity was low within the bed and high in the region
above it, to suspend the particles, so, the solids heating rate
in each zone was different. All particles within each region
were assumed spherical, and travelled at the same velocity
with no axial inter-particle conduction. The liquid in each
region was assumed well mixed with no radial temperature
gradient, and travelled at a uniform velocity. There was
no interchange of particles between the two regions but
inter-¯ uid heat transfer could occur.
Mass and energy balances were written for each zone; the
two zones were assumed to ® ll half the tube volume, and for
mass balance purposes all of the particles were assumed to
be contained in the bed. The energy balance included heat
accumulation, thermal diffusion, convective ¯ uid ¯ ow, and
heat exchange with the surroundings (wall-¯ uid, particle-
¯ uid, and ¯ uid-¯ uid heat transfer between the two zones).
The wall-¯ uid heat transfer coef® cient was arbitrarily set
at 225 Wm - 2 K- 1 whereas values of hf p were estimated
from the Ranz-Marshall correlation (equation (7)). The
¯ uid-¯ uid heat transfer coef® cient between the two zones
was also arbitrarily ® xed at 500 Wm - 2 K- 1 , to represent an
intermediate case of incomplete ¯ uid mixing, for most
studies, but the effects of setting the value to 0 and
105 Wm - 2 K- 1 were also investigated. Studies were
Trans IChemE, Vol 76, Part C, March 1998
23
conducted for a typical food processing Biot number
range of 0.1-10. The range of process parameters modelled
are summarized in Table 3.
The results showed clear differences in heating rates
between parts of the ¯ ow, and demonstrate the effects of
phase velocity and slip velocity. Phase velocity controlled
the length of the heating tube; here the process is governed
by the ¯ uid temperature, whilst slip velocity controlled the
length of the hold tube required to sterilize particles whose
heating rate was strongly dependent on hf p . Phase
temperature was also crucial; hold tube length was strongly
in¯ uenced by the temperatures at the exit of the heating
section. Equality of phase velocities was found to give the
best results but this, however, is not usually achievable in an
industrial context. The details of the results re¯ ect the case
studied, but the model does highlight the factors that
in¯ uence the process following the models of Manson and
Cullen9 and Sastry8 3 . It shows that it is not suf® cient to
consider parts of the process in isolation but rather the whole
process needs to be considered and an integrated approach
should be followed in design.
Although the model includes heat transfer coef® cient
data, it uses a number of simplifying assumptions which
may not re¯ ect the conditions of industrial processes. For
instance, the assumption of a strati® ed ¯ ow with two
separate zones each characterized by uniform velocity and
temperature pro® les is unlikely to be true in practice6 . To
extend models requires more information on realistic
velocity distributions, and realistic wall-¯ uid and ¯ uid-
¯ uid heat transfer coef® cients. This information is crucial in
determining the solids heating rate, and hence the hold tube
and the overall process length. More work is needed in this
area.
Although a number of mathematical models for hetero-
geneous aseptic food processing have been produced, they
are often incomplete. Oversimpli® cations regarding both
heat transfer and residence times mean that most models are
only suitable for very speci® c cases, i.e. where the Biot
number is high, or for plug ¯ ow. Any model should solve for
both ¯ uid and solid phases temperatures iteratively, and
incorporate different phase velocities and heat transfer
coef® cients. As accurate data is lacking for factors such as
particle concentration, the complex solid-liquid ¯ ow
pattern, and residence time distributions, most models
may be unacceptable for accurate use. The ¯ uid-particle
heat transfer coef® cient used in the models are either based
on the theoretical limit of Nu = 2, or exists in the form of a
constant value (i.e. assuming particle conduction controls
heat transfer). Similarly the wall heat transfer coef® cient is
derived from assuming either pure laminar ¯ ow in a pipe, or
entered as an arbitrary constant.
Whilst the basic approach of heat balances and conduc-
tion equations outlined is correct, accurate heat transfer
coef® cients and two-phase ¯ ow data are needed to predict
temperature distributions. The assumptions of many models
for the wall-¯ uid and ¯ uid-particle heat transfer coef® cients,
are not based on food ¯ ow observation or experimentation
and so will give model results that can only be considered
qualitative.
4.2. Modelling Studies in Process Engineering
One of the primary limitations of the work described
24 BARIGOU et al.

Table 3. Range of process parameters used in the simulation of Mankad and Fryer38.

Manipulated parameter Simulation range

Slip velocity above bed (ms- )1

10- 4- 10- 2
Slip velocity within bed (ms- 1) 0.1, 0.5, 1 times the value above bed
Solids fraction above bed negligible
Solids fraction within bed 30±50%
Fluid-¯ uid heat transfer coef® cient (Wm- 2K- 1) 0, 500, ¥ (in practice 10,000)

Property Fluid Solid

Density (kg m- 3) 1000 1000

Thermal conductivity (Wm- 1K- 1) 0.645 0.645
Speci® c heat capacity (J kg- 1 K- 1) 4184 4184
Viscosity (Pa s) 0.025 ±
Initial temperature (8 C) 15 15
Tube diameter (m) 0.075 (heat and hold sections)
Particle diameter (m) 0.01
Total mixture ¯ owrate (m3 s- 1 ) 0.001
Total delivered solids concentration 20%
Heater temperature (8 C) 150

above is the lack of knowledge of heat transfer coef® cients. position at time t,
Most models have used experimental data obtained for
isolated single particles which, as already noted, does not 3(wk)s ¶Tp ¶Tf
fully represent the heat transfer processes in such ¯ ows. One Rp (q u)s ¶rp r =R
= (wCp )f ¶x
p p
possible better approach, is to consider the ¯ owing
¶ Tf 1 ¶Tf
particulate system as a packed bed, and to produce a 2
model based on data and correlations for these types of + e kf r2 + r r , (21a)
¶t t ¶ t
systems. This is not fully accurate, since in a packed bed the
particles are stationary. However, considerable work in
process engineering has studied heat transfer and ¯ ow with boundary condition,
behaviour for high concentrations of solids in ¯ uids, albeit ¶Tf
at particle sizes, concentrations, and Reynolds numbers not - kf
¶rt rt =Rt
= Uw(Ta - Tf ), (21b)
characteristic of food ¯ ows. These models may still provide
considerable insight into heat transfer and ¯ ow behaviour, where; w is the mass ¯ owrate, Tp is the particle temperature,
and some of the data and techniques used may also be Tf is the ¯ uid temperature, Ta is the ¯ uid temperature at
adopted for food ¯ ow systems. To develop a model for food inlet, k is thermal conductivity, Cp is speci® c heat capacity,
¯ ows, it might be possible to use existing data for heat or Uw is the overall heat transfer coef® cient at the tube wall, us
mass transfer in packed beds. is the solids phase velocity, Rp is the particle radius, Rt is the
Within process engineering, heat transfer in solid-liquid tube radius, rp and rt are particle and tube radial positions
¯ ows is very important in catalytic systems and absorbers. respectively, x is axial position, and e is the bed voidage.
Many of the models and theories for predicting equipment The two equations were written in dimensionless form
sizes from heat transfer data have proved reliable. In recent and then solved by Laplace transforms and Bessel functions.
years, most processes have tended to be designed using A number of solutions for different cases were presented
computational solutions of the fundamental governing (such as small particles, no heat generation, etc.). The
equations, unlike the mainly traditional practices of the solution presented for a ® xed bed could be used without any
food industry. iterative numerical procedure, however, for moving bed
One of the ® rst relevant analytical models was developed systems an iterative solution was required.
by Amundson1 0 2 , to predict phase temperatures in ® xed and Three models describing unsteady state heat transfer in
moving beds. A two dimensional energy balance, based on packed beds were given by Wakao and Kaguei1 0 3 , using
¯ ow in a horizontal cylinder, was derived for the ¯ uid phase. energy balances for the two phases;
The solid particles were assumed spherical and their energy
balance was based on one-dimensional transient heat (i) The Schumann model, the least complex of the three,
conduction into a sphere. Internal heat generation was assumes ideal plug ¯ ow in the ¯ uid, and no thermal
included within the solids energy balance to account for heat resistance in the particle (i.e. Bi = 0). The ¯ uid energy
generation during catalytic reaction. The solids phase balance may then be written as,
energy balance was identical to equation (18a) with an
additional heat generation term, and subject to boundary ¶Tf ¶Tf hfp as
condition (18b). ¶t
= - uf ¶x - e (Cpq )f
(Tf - Ts ). (22a)
The ¯ uid phase energy balance was two-dimensional,
estimating the ¯ uid temperature at a radial, and axial The solids phase temperature is calculated using Newton’ s

Trans IChemE, Vol 76, Part C, March 1998

 HEAT TRANSFER IN TWO-PHASE SOLID-LIQUID FOOD FLOWS 25

law of heating, using a pre-determined heat transfer 5. CONCLUSIONSÐ THE NEED FOR FUTURE
coef® cient, hf p , thus, WORK
¶Ts hfp as Continuous aseptic processing of solid-liquid food
(1 - e )
¶t
= (Cp q )s
(Tf - Ts ). (22b) mixtures is an elegant alternative to canning technology.
However, the dif® culty in predicting the complex two-phase
These two equations are effectively simpli® ed versions of ¯ ow and heat transfer rates, and hence in ensuring
equations (18a) and (17). commercial sterility and optimum quality, makes it an
intricate industrial problem. The process is often subjected
(ii) The C-S model (continuous solid) develops the
to a wide distribution of particle concentration, velocities,
Schumann model slightly further. The ¯ uid energy balance
residence times, and temperatures, thereby causing a wide
is identical to that derived in the Schumann model but
and still largely unpredictable distribution of those quality
includes a thermal diffusion term; this assumption is
changes that are imparted to the food by the heat treatment.
common in packed beds. The solid particles are still
As a result, the design of such a process remains to a great
assumed to have in® nite conductivity (i.e. Bi = 0), so that
extent empirical.
each individual particle is isothermal, but a conductivity
The FDA have recently validated an aseptic process for
term (i.e. a ¶2 Ts / ¶x2 term) is included to calculate inter-
particulates, using a protocol which incorporates (i) RTD
particle heat transfer between particles in contact:
determination using the Hall effect sensor technique
for the ¯ uid, developed by CCFRA (for details see Lareo et al.6 ), (ii) a
model for the thermal behaviour of the system developed
¶Tf ¶ Tf ¶Tf
2
kf hfp as from that of Chandarana and Gavin9 8 developed by Lee
¶t
= e (Cp q )f ¶x2 - uf x - e (C q ) (Tf - Ts );
¶ p f et al.9 9 . Calculations were con® rmed by an inoculated pack
(23a) study. Recent US work reported through a series of
workshops1 1 9 ± 1 2 3 describes problems in developing and
for the solid, validating an aseptic process, and con® rms both (i) the
importance of accurate knowledge of the interfacial heat
¶Ts ks ¶2 Ts hfp as
(1 - e )
¶t
= (Cp q )s ¶x2 + (Cpq )s (Tf - Ts ). (23b) transfer coef® cient1 2 3 , and (ii) the consequences of the
incorrect choice of hf p in any model1 2 0 .
(iii) The D-C model (dispersed-continuous) is now the most Particle heat-transfer coef® cients, like particle tempera-
widely used. The model is based on the ¯ uid having tures, cannot at present be measured directly and reliably in
dispersed plug ¯ ow and the intra-particle temperature a continuous heat-hold-cool system: the main control
having radial symmetry. The solids energy balance is technique remains to be the measurement of liquid
the one dimensional transient heat conduction equation temperature. Although considerable experimental and
(equation (19)), theoretical work has been done on the particle surface
heat transfer coef® cient, applications to real food ¯ ows are
for the ¯ uid, severely limited. These limitations arise because the
experimental equipment and techniques adopted are on
¶Tf ¶ Tf ¶Tf
2
hfp as
¶t
= a f ¶x2 - uf ¶x - e (Cp q )f
Tf - Ts | r =R ;
p t
the main not representative of commercial food sterilizers.
The degree of relevance of the results to real food
(24a) processing situations vary from one study to another, as
demonstrated in Figure 1 and Table 1. The key problem is
for the solid,
that of knowing the ¯ ow ® eld round the particle; the simple
¶Tp a s ¶ r2 ¶Tp de® nition of slip, the difference between mean ¯ ow and
=
¶t R2p ¶rp
p
¶rp
, (24b) particle velocities, is not appropriate. Extensive experi-
mental data is available for stationary particles, but it is not
with boundary condition, clear how this relates to the industrial case of translating and
ks ¶ s
T rotating particles. Some progress has been madeÐ via
¶rp rp =Rp
= hfp Tf - Ts | r =R .
p p
(24c) moving thermocouples, liquid crystals, and temperature
pillsÐ to analyse the real problem: these experiments have
Apart from the inclusion of a thermal diffusion term, and the been invaluable, but more work is needed to de® ne the
absence of an external heat transfer term in the ¯ uid energy interfacial heat transfer coef® cient to a level where it can be
balance, the D-C model is identical to equations (17)±(18), used with con® dence.
which are commonly used in food processing to estimate Very little is known about the wall-¯ uid heat transfer
solid-liquid temperature pro® les. coef® cient in food processing, and in particular the effect of
These models constitute the basis for much of current particle loading. This parameter is crucial for designing the
equipment design. Due to the close similarity to an actual length of the heating tube, and hence also in¯ uences the
food sterilizer, the work of Amundson1 0 2 has strong appli- length of the holding tube. The process engineering
cability to food ¯ ow situations; modern computers can now literature is rich on this subject but, unfortunately, most of
solve the iterative equations fully. Computational solution of it is not relevant to the ¯ ow of food mixtures. Progress in
fundamental equations, which may need to be speci® cally this area has been hampered by the lack of appropriate
derived, such as those presented by Wakao and Kaguei1 0 3 , measurement techniques.
provides the best way of obtaining accurate models, as the Hard experimental data and theoretical models are still
initial assumptions serve to de® ne the model. needed to predict the fundamental parameters that in¯ uence

Trans IChemE, Vol 76, Part C, March 1998

26 BARIGOU et al.

process design. Two important areas can be identi® ed where `moving thermocouple’ technique without having the
there is a clear de® ciency of experimental data: constraining thermocouple), whilst heat ¯ ux sensors may
(i) Particle concentration effectsÐ the process engineering provide the solution to the measurement of the wall-¯ uid
literature has mainly concerned itself with packed beds, but heat transfer coef® cient. On the theoretical front, computa-
the effect of bed voidage on the particle heat transfer does tional solutions are required for the fundamental equations
not seem to have been properly investigated. On the other governing the ¯ ow and heat transfer in solid-liquid ¯ ows.
hand, food science/technology research has mainly dealt This is a much more complex problem and progress in this
with single, and often static, particles. The practical reality area is likely to be slow because of the great computational
in terms of solids concentration lies between these two dif® culty in handling multiple particle systems of this
extremes and needs to be rigorously addressed. type1 0 4 .
(ii) Fluid ¯ owrate effectsÐ solid-liquid ¯ ows in indus-
trial sterilizers6 usually correspond to tube Reynolds
numbers below 500, and particle slip Reynolds numbers NOMENCLA TURE
of less than 100. Most of the existing research, particularly as solids speci® c surface area, m2 m- 3
that reported in process engineering literature, has been Ahx heat exchanger heat transfer surface area, m2
conducted at Reynolds numbers far greater. Future research Ap particle surface area, m2
needs to be targeted at realistic food ¯ ow regimes. Aw wall heat transfer surface area, m2
Bi Biot number (hfpx k-s 1 ), -
C cook value, min
Although a number of modelling studies have been Cp speci® c heat capacity, J kg- 1 K- 1
reported they have not had a major industrial impact. dp particle diameter, m
Mathematical models for sterilizers have to be built on dt tube diameter, m
oversimplifying assumptions which make them either F sterility value, min
Fo Fourier Number (a st x- 2), -
unrealistic or suitable for only very limited cases of g acceleration due to gravity, m s- 2
practical food processing. For instance, most models adopt Gr Grashof number (gx3 j D Tq 2f l - 2 ), -
heat transfer coef® cients (¯ uid-particle and wall-¯ uid) that hfp particle convective heat transfer coef® cient, W m- 2K- 1
are largely based on inappropriate empirical relationships hw wall convective heat transfer coef® cient, W m- 2K- 1
such as single particle expressions or turbulent ¯ ow k thermal conductivity, W m- 1 K- 1
l length, m
conditions. Factors such as particle concentration, the two- mp particle mass, kg
phase ¯ ow pattern, and residence time distribution have not np number of particles, -
been considered due to the poor current understanding of the Nu Nusselt number (hfpx k-f 1 ), -
complex physics of such ¯ ows. The often used assumption P pressure, Pa
PeÂclet Number (uf x a - 1 ), -
of no slip between particle and ¯ uid (i.e. Nu = 2) is clearly Pe
Pr Prandtl number (Cpl k-f 1 ), -
too conservative, but does at least represent a minimum safe Q volumetric ¯ owrate, m- 3 s- 1
value for the processing of the particle phase, although it r radius, m
may by reducing the heat transfer between particle and Re tube Reynolds number (q fumdt l - 1 ), -
liquid, lead to an overestimate of liquid temperature1 2 0 . Rep particle Reynolds number (q fufdp l - 1 ), -
Reslip particle slip Reynolds number (q fuslipdp/l - 1 ), -
Particle slip is an important characteristic of solid-liquid Rex rotational Reynolds number (Rex = 2q f x R2p l - 1 ), -
food ¯ ows and will enhance ¯ uid-particle heat transfer Rp particle radius, m
considerably above the Nu = 2 limit. Particle rotation will rp radial position in particle, m
also enhance heat transfer; it is not known how important rt radial position in tube, m
Rt tube radius, m
this will be under conditions of moderate to high solids s relative density, -
loadings. At this stage it might be reasonable to assume that T temperature, K
heat transfer effects due to particle rotation in food ¯ ows are t time, min or s
not signi® cant; again this will result in too low a heat Tcref cook reference temperature, 8 C
transfer coef® cient. Tfo original ¯ uid temperature, 8 C
Tfref sterility reference temperature, 8 C
The effects of particle-particle interactions are not well Th heating temperature, 8 C
understood and require further extensive research. These Ti initial particle temperature, 8 C
interactions can give rise to ¯ uid streamline disturbances Tps particle surface temperature, 8 C
which may be superimposed on the ¯ ow ® eld around Tw wall temperature, 8 C
u velocity, m s- 1
successive particles and, depending on the Reynolds ufmax maximum ¯ uid velocity, m s- 1
number, can give rise to enhanced particle heat transfer ufx ¯ uid velocity in x-axis vector, m s- 1
coef® cients. Furthermore, where particle concentration is ufy ¯ uid velocity in y-axis vector, m s- 1
high, ¯ uid channelling can occur and this can signi® cantly Uhx heat exchanger overall heat transfer coef® cient, W m- 2K- 1
affect the heat transfer coef® cient. um mean mixture ¯ ow velocity, m s- 1
uslip slip velocity, m s- 1
A combination of experimental and theoretical work Uw overall heat transfer coef® cient at tube wall, W m- 2K- 1
relevant to real solid-liquid ¯ ow situations is needed to w mass ¯ ow rate, kg s- 1
identify the optimal conditions for the design and operation x characteristic length, m
of continuous aseptic processes. Future developments in zc cook thermal death time constant, 8 C
zf sterility thermal death time constant, 8 C
instrumentation will probably provide the necessary
information on the important heat transfer parameters.
Subscripts
For instance, improved remote temperature sensor methods f ¯ uid
will give much better data on the particle heat transfer p particle
coef® cient (for example, using the methodology of Sastry’ s s solids

Trans IChemE, Vol 76, Part C, March 1998

 HEAT TRANSFER IN TWO-PHASE SOLID-LIQUID FOOD FLOWS
Greek symbols
a thermal diffusivity, m2 s- 1
e bed voidage, -
j coef® cient of cubical expansion, K- 1
l dynamic viscosity, Pa s
l p interfacial viscosity, Pa s
m kinematic viscosity, m2 s- 1
q density, kg m- 3
x angular velocity, s- 1
Abbreviations
FDA Food and Drug Administration
RTD Residence Time Distribution
CCFRA Chipping Campden Food Research Association
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ACKNOWLEDGEMENTS
SMs PhD work was funded as part of a DTI Link scheme on food
processing, in collaboration with Campden Food and Drink Research
Association and sponsored by Unilever UK Central Resources Ltd, APV
Baker Ltd, Alfa Laval Pumps Ltd, HJ Heinz Co Ltd, Master Foods, and
Nestle UK Ltd.
ADDRESS
Correspondence about this paper should be addressed to Dr M. Barigou,
School of Chemical Engineering, University of Birmingham, Edgbaston,
Birmingham B15 2TT, UK.
The manuscript was received 25 July 1997 and accepted for publication
after revision 5 January 1998