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# Institution of Chemical Engineers
Trans IChemE, Vol 80, Part B, May 2002

CALCULATION AND CONSIDERATION OF THE LEWIS

NUMBER FOR EXPLOSION STUDIES
A. CLARKE
Wolfson School of Mechanical and Manufacturing Engineering, Loughborough University, Loughborough, UK

W
hen a laminar  ame front becomes cellular, the  ame front area increases and the
rate at which the unburnt gases are consumed is increased. If this is not taken into
account when modelling vented or non-vented explosions, the pressures that vessels
containing explosions are subject to can be greatly under-predicted.
For most explosion models, hydrodynamic instabilities are considered as the only driving
force for the formation of cellular  ames. This paper shows that the transition to cellular  ame
propagation can occur earlier due to thermo-diffusive instabilities.
To predict when thermo-diffusive instabilities should be considered as the main driving force
for cellular  ame transition, the Lewis number of the reactant mixture should be compared to a
critical value.
Calculations of the Lewis number for a range of different fuel=air mixtures that are in common
use are presented. The fuels studied are methane, ethane, propane and n-butane. For each of these
fuel=air mixtures the critical Lewis number was evaluated using an expression from asymptotic
analyses. It is shown that the critical Lewis number based on this type of analysis is under-
predicted. This is because the  ame thickness is not included. It is proposed that a modiŽ ed form
of the critical Lewis number be used which is greater by an order of 1=Zeldovich number.

Keywords: Lewis number calculation; hydrodynamic instabilities; thermo-diffusive instabil-

ities; cellular  ames; explosion protection.

INTRODUCTION instabilities; and 2) thermo-diffusive instabilities. These

During a fully conŽ ned or vented explosion it is imperative
that engineers can predict the change in pressure that a
pressure vessel, or pipe, will be subjected to with respect
to time. Over the years a number of mathematical models
have been proposed which predict the internal pressure as a
function of time and mixture composition and have been
based on the rate of conversion of the unburnt mixture to the
burnt state1–3.
In predicting the pressure=time history during an explo-
sion, it is common to derive an expression that relates the rate
of change of the unburnt gases to burnt gases as a function of
the laminar burning velocity and  ame front area:
dmb
ˆ ru Af Su
dt
Care must be taken when using equation (1) as it can only
be applied when the  ame shape is known, or is assumed to
be spherical.
During combustion a number of instabilities can occur
that will alter the shape of the  ame and can lead to loca-
lized  ame acceleration which in turn will produce cellular
type  ame propagation. If this fact is not included in the
combustion model, the predicted pressure=time history will
be under-predicted and could constitutea major safety hazard.
When considering explosions, the two main types of  ame
instabilities that should be considered are: 1) hydrodynamic
instabilities are outlined below.
As combustion proceeds, the unburnt gases react and
form the burnt gases which have a much lower density. The
differences in density between the burnt and unburnt gases,
characterized by the expansion ratio a, is the driving force
for the hydrodynamic instabilities, and affects all  ames
irrespective of fuel composition and mixture strength. The
transition to cellular  ame propagation, via the hydrody-
namic instability mechanism, can be predicted using the
theory of Istraov and Librovich4. In this theory the  ame
becomes cellular when the product of the Reynolds and
Prandtl numbers reaches a critical value. It should be noted
that the product of the Reynolds and Prandtl numbers is the
deŽ nition of the  ame Peclet number used in many stability
…1† studies5. Groff6 showed that for lean and stoichiometric
mixtures of propane=air, the critical Reynolds number Re*
could be correlated in a linear fashion to the expansion ratio.
Using a linear curve Ž t Chippett2 obtained the following
relationship:
Re¤ ˆ 155555a ¡ 166667 …2†
where the Reynolds number is based on the  ame radius and
the laminar burning velocity.
However, if this stability criterion is applied to rich
n-butane=air  ames, problems are soon observed. Figure 1
shows the experimental results of laminar burning velocity

135
136
Figure 1. Laminar burning velocity v=s  ame radius (n-butane=air j ˆ 1.5).
against burnt gas radius for a rich (F ˆ 1.5) n-butane=air
mixture for a non-vented explosion7. Also shown are the
predicted values of the laminar burning velocity based on a
pressure and temperature power law8.
³ ´1:45 ± ²
T p ¡0:233
Su …P; T † ˆ 42:1 …3†
298 1:0
As combustion proceeds, it can be seen that the experi-
mental laminar burning velocity data starts to deviate from
the predicted values at a  ame radius of approximate-
ly 65 mm. The expansion ratio at this point is 0.145. For
this expansion ratio, equation (2) yields a critical Reynolds
number of 5888. However, the experimental value of the
Reynolds number is only 1665. Clearly, if transition to cel-
lular  ame conditions were based on the previous work6
the predicted pressures would be signiŽ cantly in error due
to the enhanced burning velocities.
To explain the early transition to cellular  ames, consid-
eration of thermo-diffusive instabilities is required. This
instability is driven by differences between the diffusivities
of mass and heat and is quantiŽ ed by the Lewis number Le
deŽ ned in equation (4):
k thermal diffusivities are not taken into account, the risk of
Le ˆ
ru cp D
This type of instability can, under certain circumstances,
either stabilize the  ame until hydrodynamic instabilities
become dominant, or can promote the onset of cellular  ame
propagation before the critical Re value has been reached.
Figure 2 schematically shows the  ame front as a reaction
sheet. It can be considered as a sink for reactants and a
source for heat. If the Lewis number is unity, i.e. normally
diffusing reactants, then at the bulge A, the increased heat
loss from the reaction sheet is balanced by the enhanced rate
of diffusion of the reactants. The net result is that there is
no change in the  ame temperature, the  ame proceeds
normally and the perturbation remains unchanged.
If the Lewis number is greater than unity, i.e. weakly
diffusing reactants, there is an increase in the heat trans-
ferred to the unburnt charge and the  ame temperature at the
apex of bulge A will be reduced. This reduction in the  ame
temperature reduces the  ame speed. For the concave part of
CLARKE
Figure 2. Schematic illustration showing the mechanisms of thermo-
diffusive instabilities.
the  ame, point B, the increased heat transfer to the unburnt
gases is focused and the unburnt gases are preheated, which
increases the  ame speed. In this case the thermo-diffusive
instabilities stabilize the  ame until the hydrodynamic in-
stabilities become dominant and the  ame becomes cellular.
This is the condition that existed for the test cases used by
Groff 6 to predict cellular  ames.
For the case where the Lewis number is less than unity, i.e.
strongly diffusing reactants, the  ame temperature at point A
is greater than the ideal  ame temperature due to the in-
creased reactant diffusion to the  ame front. This causes the
 ame speed to increase. Due to this increased  ame speed
at the apex of the  ame, the tip of the  ame propagates further
into the unburnt gases until cellular  ame propagation is
observed. For these conditions the  ame progresses to
cellular propagation earlier than if the mechanism were
purely hydrodynamic. This is the driving force for the rich
n-butane=air  ame to become cellular at a much lower
Reynolds number than predicted by Groff 6.
Clearly, if the effects of imbalances in the mass and
…4† major injury or death due to under-prediction of explosion
pressures is signiŽ cantly increased.
Therefore it is important to be able to calculate the
magnitude of the Lewis number of the unburnt mixture and
compare it to a critical value to see if the  ame will become
cellular based on the critical Reynolds number or if early cel-
lular propagation will take place. This paper presents the
key references to allow calculation of the Lewis number for
non-polar gaseous combustible mixtures, and proposes a
critical Lewis number below which the  ame will attempt to
become cellular prior to the  ame reaching the critical
Reynolds number.
CALCULATION OF THE MIXTURE
LEWIS NUMBER
The calculation of the mixture density and isobaric heat
capacity in the study were based on the ideal gas theory
for mixtures and can be found in most textbooks on
Trans IChemE, Vol 80, Part B, May 2002
 CALCULATION AND CONSIDERATION OF THE LEWIS NUMBER FOR EXPLOSION STUDIES 137

thermodynamics9. However, the calculation of the thermal Table 2. CoefŽ cients for determination of the collision integral11.
conductivity and mass diffusion coefŽ cient are considerably
more complex and are detailed below. A B C D a b w g

1.06036 0.193 1.03587 1.76474 0.1561 0.47635 1.52996 3.89411

THERMAL CONDUCTIVITY
To allow the thermal conductivity of the combustible
mixture to be determined, the thermal conductivities of the MASS DIFFUSION COEFFICIENT
individual gaseous components have to be calculated at the
system conditions. At low to moderate pressures (between The mass diffusion coefŽ cients of the individual compo-
1 ¹ 10 bar) the effects of pressure are relatively small and nents are calculated from the Chapman Enskog equation10
for this study are neglected with errors expected to be less (derived from the Boltzman equation):
Á ! s 






than 5%. The thermal conductivity for the individual 1:8583E ¡ 3 3=2 1 1
chemical species were determined as a function of tempera- Di;j ˆ T ‡ …10†
ture only for a pressure of 1 bar. Two expressions were ps2i;j OD Mi Mj
employed depending on which species was being evaluated. where the mass diffusion coefŽ cient is in W mK¡1.
ki ˆ a ‡ bT ‡ cT 2 ‡ dT 3 …5a† For the diffusion collision integral, the relationship initi-
ally proposed by NeuŽ eld et al.11 was employed.
aT b A B C D
ki ˆ ³ ´ …5b† OD ˆ ‡ a ‡ ‡ ‡
c d …T † exp…bT ‡ † exp…wT ‡ † exp…gT ‡ †
1‡ ‡ 2
T T …11†
The coefŽ cients for equations (5a) and (5b), to yield the The coefŽ cients for the diffusion collision integral are
thermal conductivity in cm2 s¡1, are given in Table 1. contained within Table 2.
To estimate the thermal conductivity of the mixture, the Where the temperature T ‡ ˆ T =…e=k†ij and …e=k†ij is the
Waailjewa equation10 was employed: geometric mean value of the individual values of …e=k† for
Xn yk each individual constituent molecule.
kmix ˆ Pn i i …6† Data for …e=k† and s for the fuels and oxidants are
jˆ1 yj Aij
iˆ1
supplied in Table 3. These data are based on the Lennard-
where Aij is deŽ ned as: Jones (6–12) potentials calculated using viscosity data. It
0 Á !1=2 Á !1=4 12 should be noted that this calculation is only suitable for
mixtures of non-polar gases. If polar mixtures of gases are
@1 ‡ ktri Mi A under examination the author recommends the use of the
ktrj Mj Stockmayer (12-6-3) potentials. This is due to the effects of
Aij ˆ Á Á !!1=2 …7† the di-polar moments on the diffusion properties of the
Mi mixtures. For further details the reader is advised to review
8 1‡
Mj the paper by Paul and Warnatz12.
Once the binary diffusion coefŽ cients for the various
In equation (7), ktr is the monatomic value of the individual combinations of gases have been calculated, a method for
translational thermal conductivity determined using equa- determining the effective diffusion coefŽ cient of the deŽ -
tion (8). cient species into the remaining mixture had to be selected.
ktri Gj ‰exp…0:0464Tri † ¡ exp…¡0:2412Tri †Š There are a number of different methods for calculating
ˆ …8† the effective diffusion coefŽ cient, all of which are derived
ktrj Gi ‰exp…0:0464Trj † ¡ exp…¡0:2412Trj †Š
from the solution of the Stefan-Maxwell diffusion equa-
where Tri is the reduced temperature of the ith component, tions10,13,14. As there are very little experimental data to
T=Tcrit. Gi is the reduced inverse thermal conductivity of validate the different methods, the method proposed by
species i and is deŽ ned in equation (9): Wilke13 was employed in this study.
( )1=6 0 1
Tcrit;i Mi3 BXn
yj C
Gi ˆ 210 …9†
P 4crit;i Di;mix ˆ B
@
C …12†
D A
jˆ1 i;j
For the case where i ˆ j, the value of Aij ˆ 1.0. …j6ˆi†

Table 1. CoefŽ cients for thermal conductivity calculations10,21.

Formula Name Equation a B c d T range (K) Ref.

O2 Oxygen 5a ¡ 3.273E¡ 4 9.966E¡ 5 ¡ 3.743E¡ 8 9.732E¡ 12 115 to 1470 10

N2 Nitrogen 5a 3.919E¡ 4 9.816E¡ 5 ¡ 5.067E¡ 8 1.504E¡ 11 115 to 1470 10
CH4 Methane 5a ¡ 1.869E¡ 3 8.727E¡ 5 1.179E¡ 7 ¡ 3.614E¡ 11 273 to 1270 10
C2H6 Ethane 5a ¡ 3.174E¡ 2 2.201E¡ 4 ¡ 1.923E¡ 7 1.664E¡ 10 273 to 1020 10
C3H8 Propane 5a 1.858E¡ 3 ¡ 4.698E¡ 6 2.177E¡ 7 ¡ 8.409E¡ 11 273 to 1270 10
C4H10 n-Butane 5b 5.1094E¡ 2 4.5253E¡ 1 5.4555E‡ 3 1.9798E‡ 6 273 to 1000 21

Trans IChemE, Vol 80, Part B, May 2002

138 CLARKE

Table 3. Lennard-Jones 6–12 potential based on viscosity data22.

Formula Name s=10¡10 m e=k, K

Air Air 3.711 78.6

O2 Oxygen 3.467 106.7
N2 Nitrogen 3.798 71.4
CH4 Methane 3.758 148.6
C2H6 Ethane 4.443 215.7
C3H8 Propane 5.118 237.1
C4H10 n-Butane 4.687 531.4

CALCULATION OF THE CRITICAL

LEWIS NUMBER
Generally, a Lewis number of less than unity is consid-
ered the requirement for cellular  ames to begin. However
using asymptotic analysis15 for an adiabatic  ame, the
instability was found to occur below unity:
2
Le¤ µ 1 ¡ …13† Figure 3. Lewis numbers and critical Lewis numbers for methane=air
b mixture at 1 bar and 298 K.

where b is the Zeldovich number deŽ ned as:

Ea …Tb ¡ Tu †
bˆ
Ro Tb2
Values of Tb were obtained from a chemical equilibrium
code assuming constant pressure combustion16. The activa-
tion energies were obtained from single step reaction rate
parameters17, and a value of 30 kcal gmol¡ 1 was employed
for all calculations.
However, as the  ame front was considered to be an
inŽ nitely thin density discontinuity, the asymptotic analysis
under-predicts the critical Lewis number by an amount of
the order of (1=b)18. Hence, for this study, a second critical
Lewis number Le¤2 was deŽ ned as:
1 employed, the Lewis numbers for the rich mixtures tend
Le¤2 µ 1 ¡
b
From these Ž gures it is seen that for lean and stoichio-
…14† metric mixtures the Lewis number based on air as a single
substance is in rough agreement with the Lewis number
based on the limiting (deŽ cient) species. However when the
Lewis numbers for the rich mixtures are examined, consid-
erable differences are evident.
Using the Lewis number based on the limiting (deŽ cient)
species, Di,mix, there is an awkward jump as the mixture
passes through the stoichiometric point. To overcome this
jump condition, Joulin and Mitani19 proposed an expression
based on asymptotic analysis of a two reactant  ame which
weighted the Lewis numbers for both limiting reactants
conditions. This allows a smooth transition of the Lewis
number from weak to rich conditions. However, when
…15†

RESULTS AND DISCUSSION

Using the methods described in the previous sections of
this paper, the mass and thermal diffusivities for combus-
tible mixtures of methane, ethane, propane and n-butane air
mixtures were determined. From these calculations the
actual and critical Lewis numbers were calculated.
Two Lewis numbers for each of the mixtures considered
are presented. The Ž rst treats air as a single ideal gas and
hence the binary mass diffusion coefŽ cient could be
employed. The second is based on the diffusion of the
deŽ cient (or limiting) species diffusing into the remaining
mixture, e.g. fuel diffusing into oxygen and nitrogen for the
lean and stoichiometric mixtures, and oxygen diffusing into
fuel and nitrogen for rich mixtures.
Figures 3 to 6 shows the two Lewis numbers for methane=
air, ethane=air, propane=air and n-butane=air mixtures re-
spectively. For these Ž gures the thermodynamic conditions
were a pressure of 1 bar (abs) and a temperature of 298 K.
Also shown on Figures 3 to 6 are the critical Lewis numbers
for the respective fuel air mixtures using equations (13) Figure 4. Lewis numbers and critical Lewis numbers for ethane=air mixture
and (15). at 1 bar and 298 K.

Trans IChemE, Vol 80, Part B, May 2002

 CALCULATION AND CONSIDERATION OF THE LEWIS NUMBER FOR EXPLOSION STUDIES
Figure 5. Lewis numbers and critical Lewis numbers for propane=air
mixture at 1 bar and 298 K.
more towards unity. For this reason, the method was not
employed in this study.
Figure 3 shows the results for methane=air mixtures which
are known to be relatively stable. The calculated Lewis
number is greater than both the critical Lewis numbers for
all mixtures. For this fuel one could expect that cellular  ame
transition would occur due to hydrodynamic instabilities
only and that thermo-diffusive instabilities are negligible.
For mixtures using ethane and propane as the fuel, the
Lewis numbers based on the deŽ cient species for rich
mixtures lie between the two critical Lewis number values.
This is shown in Figures 4 and 5. As cellular  ames
have been observed in small combustion vessels with rich
propane=air mixtures, at relatively low Reynolds numbers,
it can be argued that the critical Lewis number should
be based on equation (15) rather than equation (13).
Figure 6. Lewis numbers and critical Lewis numbers for n-butane=air
mixture at 1 bar and 298 K.
Trans IChemE, Vol 80, Part B, May 2002
139
For the rich n-butane=air mixtures in Figure 6, the Lewis
number of the mixture was very close to the critical Lewis
number using equation (13). However for mixtures with an
equivalence ratio of 1.1, the actual Lewis number is greater
that the critical Lewis number. As cellular  ames were
observed for this mixture with low Reynolds numbers, it
can again be concluded that the critical Lewis number for
explosion studies should be based on equation (15).
For the fuel=air mixtures considered in this study, cellular
 ame transition will occur in lean and stoichiometric
mixtures when the critical Reynolds number is attained.
However for rich mixtures the Lewis number should be
determined and compared with the critical Lewis number to
see if early transition will occur. These results are in agree-
ment with the classic work of Markstein20 on cellular  ames.
The solid line on Figures 3 to 6 shows the critical Lewis
number for each mixture considered. For mixtures with a
Lewis number above this solid line, transition to cellular
 ames will be via the hydrodynamic instability. For mixtures
with a Lewis number on or below this line, the transi-
tion mechanism will be driven by the thermo-diffusive
instabilities.
The results presented allow the combustion modeller to
determine quickly whether the assumption of unity Lewis
number is a valid assumption. A critical Lewis number
which is higher than that obtained from asymptotic analysis
is proposed. This will allow the prediction of which
mixtures will become cellular based on the hydrodynamic
theory and which will become cellular earlier. This will aid
in the safe design of vented and non-vented pressure vessels.
CONCLUSIONS
(1) Lewis number calculations for mixtures of methane=air,
ethane=air, propane=air and n-butane=air have been
presented.
(2) When calculating the Lewis number of a combustible
mixture, the mass diffusion coefŽ cient must be based on
the deŽ cient species and air cannot be treated as a single
component of the mixture.
(3) The critical Lewis number should be considered to be
1-1=b rather than 1-2=b. This is due to the asymptotic
analysis, originally employed, not including the thick-
ness of the reaction sheet.
(4) Mixtures with a Lewis number lower than the critical
Lewis number will become cellular at much lower  ame
Reynolds numbers due to thermo-diffusive instabilities.
This is important when designing safety systems into
pressure vessels where there is an explosion potential.
(5) When calculating the pressure rise in a vented or
non-vented vessel, the transition to cellular  ame propa-
gation must include consideration of the Lewis number.
(6) The results presented allow the combustion modellers to
evaluate whether the unity Lewis number assumption is
valid.
NOMENCLATURE
a,b,c,d,e coefŽ cients in equations (5a) and (5b)
Af  ame surface area
Ai,j deŽ ned in equation (7)
cp speciŽ c heat at constant pressure
Di,j binary diffusion coefŽ cient of species i and j
140 CLARKE

Di,mix diffusion coefŽ cient of the deŽ cient species into remaining 5. Bradley, D., Sheppard, C. G. W., Woolley, R., Greenhalgh, D. A. and
mixture Lockett, R. D., 2000, The development and structure of  ame instabil-
Ea activation energy ities and cellularity at low Markstein numbers in explosions, Combus-
ki Boltzman constant tion and Flame, 122: 195–209.
ki thermal conductivity of species i 6. Groff, E. G., 1982, The cellular nature of conŽ ned spherical propane-air
ktr monatomic value of the individual translational thermal  ames, Combustion and Flame, 48: 51–62.
conductivity 7. Clarke, A., 1994, DPhil Thesis: Measurement of Laminar Burning
Le Lewis number Velocity of Air=Fuel=Diluent Mixtures in Zero Gravity (Oxford
Le* critical Lewis number University).
m mass 8. Clarke, A., Stone, R. and Beckwith, P., 2001, Measurement of the
M molar mass laminar burning velocity of n-butane and isobutane mixtures under
Ma Markstein number micro-gravity conditions in a constant volume vessel, Journal of the
p absolute pressure Institute of Energy, 74: 70–76.
Pe Peclet number 9. Cengal, Y. A. and Boles, M. A., 2001, Thermodynamics: An Engineer-
Pr Prandtl number ing Approach (McGraw Hill).
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Re* critical Reynolds number 11. NeuŽ eld, P. D., Janzen, A. R. and Aziz, R. A., 1972, Journal of
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yi mole fraction of species i 14. Smith, I. W. and Taylor, R., 1983, Film model for multicomponent mass
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Subscripts tion (Oxford University Press, Oxford).
b burnt 19. Joulin, G. and Mitani, T., 1981, Laminar stability analysis of two-
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ADDRESS
Correspondence concerning this paper should be addressed to Dr A.
Clarke, Wolfson School of Mechanical and Manufacturing Engineering,
Loughborough University, Loughborough LE11 3TU, UK. E-mail:
A.Clarke@lboro.ac.uk
The manuscript was received 22 October 2001 and accepted for
publication after revision 5 April 2002.

Trans IChemE, Vol 80, Part B, May 2002