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Combust i on Theory and Model l i ng
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A mat hemat i cal model of hot spot
condensed phase i gni t i on i n t he
presence of a compet i t i ve endot hermi c
react i on
A. Hmai di
a
, A. C. McInt osh
b
& J. Br i ndl ey
c
a
Cent r e f or t he st udy of Comput at i onal Fl ui d Dynami cs
b
Ener gy and Resour ces Resear ch Inst i t ut e
c
School of Mat hemat i cs, Uni ver si t y of Leeds, Leeds, LS2 9JT, UK
Avai l abl e onl i ne: 27 Oct 2010
To ci t e t hi s art i cl e: A. Hmai di , A. C. McInt osh & J. Br i ndl ey ( 2010) : A mat hemat i cal model
of hot spot condensed phase i gni t i on i n t he pr esence of a compet i t i ve endot her mi c r eact i on,
Combust i on Theor y and Model l i ng, 14: 6, 893- 920
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Combustion Theory and Modelling
Vol. 14, No. 6, 2010, 893920
A mathematical model of hotspot condensed phase ignition in the
presence of a competitive endothermic reaction
A. Hmaidi
a
, A.C. McIntosh
b
and J.Brindley
c
a
Centre for the study of Computational Fluid Dynamics;
b
Energy and Resources Research Institute;
c
School of Mathematics, University of Leeds, Leeds LS2 9JT, UK
(Received 12 May 2009; nal version received 29 July 2010)
We consider the propagation of a combustion front resulting from the gasless com-
bustion of a condensed state fuel. The propagation of the front, essentially a premixed
laminar ame, is supported by an exothermic reaction subject to possible heat loss
through a competitive endothermic reaction. The dynamics of the endothermic process
inducing the heat loss strongly depend on the temperature and the local fuel concen-
tration. Through an analysis based on high activation energy, the steady-state values of
the nal burnt temperature as well as the burning velocity are obtained, and the control
parameters are identied. Using a linear perturbation method, we assess the stability of
the propagating front and obtain a condition for oscillatory behaviour. The critical pa-
rameter values for the transition fromsteady to oscillatory burning speeds are identied.
The results represent a generalization of those obtained by Matkowsky and Sivashinsky
to include the effects of heat loss induced by a competitive endothermic reaction.
Keywords: gasless combustion; large activation energy asymptotics; ame propagation;
heat loss; competitive reaction
1. Introduction and motivation
In condensed phase combustion problems one usually distinguishes between two kinds of
behaviour. In the rst type, combustion takes place in two steps, in which total or partial
gasication of the condensed phase is followed by burning of the gaseous vapours. In the
second type, gasless combustion takes place in the solid itself and there are no gaseous
combustion products.
In this second case the combustion reaction sustains the propagation of a temperature
front separating the high temperature combustion products from the low temperature fuel.
This front propagation is described by a set of reaction-diffusion equations for the tem-
perature and for the fuel concentration. As there are no gaseous combustion products, the
fuel diffusion coefcient is set to zero. Previous work [1] has shown that, for a single,
exothermic, reaction, the front velocity may have periodic pulsations and the cause of
these pulsations was attributed to the absence of fuel diffusion. A similar model has been
analysed by Matkowsky and Sivashinsky [2], where it was shown that a solution exhibiting
a periodically pulsating, propagating reaction front arises as a Hopf bifurcation from a
solution describing a uniformly propagating front.

Corresponding author. Email: hmaidi ayoub@yahoo.com

ISSN: 1364-7830 print / 1741-3559 online
C
2010 Taylor & Francis
DOI: 10.1080/13647830.2010.519050
http://www.informaworld.com
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894 A. Hmaidi et al.
Here we consider the propagation of a ame in a condensed phase fuel in which the
driving exothermic reaction is subject to possible heat loss through an endothermic reaction.
In contrast to the work of Simon et al. [3] we assume that the endothermic reaction consumes
part of the fuel, and hence represents a competitive chemical pathway [4]. Numerous
previous studies have considered heat loss due to physical processes such as radiation or
conduction [1, 5]. The removal of heat was usually modelled by cooling linearly dependent
on temperature through a heat transfer parameter. As demonstrated in [1], the quenching of
the combustion waves is abrupt, occurring at some critical value of the heat loss parameter.
In our case, the situation is very different, as the kinetics of the endothermic process inducing
the heat loss strongly depend on both the temperature and the local fuel concentration.
It is possible that the exothermic and the endothermic reactions are coupled in either
a competing way or in a parallel way [4]. In this paper, in contrast to the work of Simon
et al. [3], we focus on the competing case, in which both exothermic and endothermic
reactions feed on the same fuel source.
Through an analysis based on high activation energy asymptotics [6], the steady-state
values of the nal burnt temperature and burning velocity are obtained and the control
parameters are identied. Using a linear perturbation method, we then obtain a stability cri-
terion for the front propagation, and establish conditions for possible oscillatory behaviour
which agree in the limiting case of vanishing endothermic effects with those obtained by
Matkowsky and Sivashinsky [2]. The results of numerical integration of the full equations
show good agreement with the analysis.
2. Problem description and mathematical modelling
2.1. Mathematical model
We consider a system of reaction-diffusion equations describing the combustion of a solid
fuel. We assume that the fuel undergoes two competitive reactions, one exothermic and one
endothermic.
The endothermic reaction induces a heat loss and is described by the parameters E
1
,
A
1
and Q
1
which are, respectively, the activation energy, the pre-exponential factor and
the heat release in the reaction. The exothermic reaction sustains the combustion and is
described by the parameters E
2
, A
2
and Q
2
.
Note that the exothermic reaction has a negative reaction enthalpy, i.e. a positive heat
release Q
2
> 0, whereas the endothermic reaction has a negative exothermicity Q
1
< 0.
The governing equations for this system are the heat and mass balance equations
[1] accounting for the reaction-diffusion of a solid fuel subject to an exothermic and an
endothermic chemical process:
c
p
T

2
T

2
+
_
Q
1
A
1
e

E
1
RT

+Q
2
A
2
e

E
2
RT

_
C

(1)

=
_
A
1
e

E
1
RT

+A
2
e

E
2
RT

_
C

. (2)
Here T

and C

, respectively, denote the temperature and fuel mass fraction. and

denote
the time and space coordinates. is the density, is the thermal conductivity and c
p
is the
heat capacity at constant pressure of the fuel. R denotes the universal gas constant.
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Combustion Theory and Modelling 895
In order to study the behaviour of a moving ame front, it is convenient to use a frame
of reference moving with the front. By transforming to a travelling coordinate frame,
=

+( ) (3)
= (4)
the partial derivatives are transformed to

(5)

. (6)
Our approach is to regard the exothermic reaction as the initially dominant process and
we let T

0
and T

ad
denote, respectively, the initial and the adiabatic burn temperature, i.e.
assuming no endothermic reaction pathway
T

ad
= T

0
+
Q
2
C
0
c
p
(7)
where C
0
denotes the initial fuel mass fraction.
An important parameter is the reduced activation energy, , dened by
=
E
2
RT

ad
. (8)
We rst address the possibility of a steady propagation front [5], and, if V is a steady-state
ame front velocity, we can introduce the non-dimensional pre-exponential term :
=

c
p
V
2
A
2
e

. (9)
Further, we introduce the non-dimensional variables
x =
c
p
V

, t =
c
p
V
2

, =

V
, T =
T

ad
, (10)
and parameters
f =
E
1
E
2
, B =
A
1
A
2
e
(1f )
, q
i
=
Q
i
c
p
T

ad
, i = 1, 2 (11)
to obtain the non-dimensional version of the reaction-diffusion system (1) and (2), referred
to a frame of reference xed in the front, as
T
t
+
T
x
=

2
T
x
2
+
_
q
1
B

e
f (1
1
T
)
+q
2
e
(1
1
T
)
_
C (12)
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896 A. Hmaidi et al.
C
t
+
C
x
=
_
B

e
f (1
1
T
)
+e
(1
1
T
)
_
C. (13)
2.2. Large activation energy and ordering of the endothermic terms
We assume that the exothermic reaction has a high activation energy E
2
, i.e.
1. (14)
Furthermore, the ame structure is presumed to consist of three zones [5]: a preheat zone,
a reaction zone and an equilibrium zone. We will use the subscripts p to denote preheat
zone, r to denote reaction zone and e to denote equilibrium zone.
(1) The preheat zone is presumed to be of thickness of order unity and to be chemically
inert, i.e. the rates of chemical reactions are assumed to be negligibly small. To describe
the steady increase of the temperature T
p
we use the following series expansion
T
p
(x) = T
(0)
p
(x) +
1

T
(1)
p
(x) + (15)
(2) The thin reaction zone of thickness of order O(
1
) is dominated by the reaction-
diffusion process and involves very large reaction rates. To describe this very thin
zone, we introduce the stretched space coordinate x, and introduce a series
expansion for the temperature and fuel in the reaction zone as
T
r
(x) = 1
1

()
1

1
() + (16)
C
r
(x) = C() +
1

C
1
() + (17)
Note that in terms of the coordinate , the reaction zone extends over the domain
[, +].
(3) The equilibrium zone, which is the postame zone, is assumed to be of thickness of
order unity as well as chemically inert since the fuel is totally consumed in the reaction
zone. The temperature T
e
is the nal burnt temperature T
b
T
e
(x) = T
(0)
e
(x)
1

T
(1)
e
(x) (18)
Furthermore, we assume that the exothermic reaction remains dominant and that the en-
dothermic reaction can be considered as a perturbation of order O(
1
) inducing a small
heat loss in the reaction zone.
The assumption of an O(
1
) heat loss is related to three important conditions:
(1) the exothermic reaction has at least a lower activation energy than the endothermic
reaction, viz.
f
E
1
E
2
1; (19)
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Combustion Theory and Modelling 897
(2) the non-dimensional group relating the pre-exponential factors and activation energies
is such that
B
A
1
A
2
e
(1f )
O(1); (20)
(3) the exothermicities q
1
and q
2
are of the same order of magnitude.
These assumptions ensure that the order of the endothermic terms in Equations (12) and
(13) is O(
1
). Also we assume that is O() and write it as
L. (21)
Far ahead in the preheat zone, we have T

= T
0
and C

= C
0
. In the equilibrium zone, we
expect that the fuel is totally consumed, i.e. C

= 0 and that the ame temperature reaches

its equilibrium value T

b
T

ad
. We anticipate the heat loss due to the endothermic reaction
to be O(
1
).
Since we normalize with the adiabatic burnt temperature T

ad
, the boundary conditions
for the temperature and fuel mass fraction across the whole region are:
x : T = T
0
, C = C
0
(22)
x +: T = 1
h

, C = 0 (23)
where h/accounts for the heat loss due to the endothermic reaction. As the fuel undergoes
two competing chemical pathways, the value of the heat loss is not a priori known, but is a
derived quantity.
3. Steady-state analysis
In this section, we focus on steady-state solutions of the reaction-diffusion system[1] which
is described by
dT
dx
=
d
2
T
dx
2
+
_
q
1
B

e
f (1
1
T
)
+q
2
e
(1
1
T
)
_
C (24)
dC
dx
=
_
B

e
f (1
1
T
)
+e
(1
1
T
)
_
C. (25)
3.1. Preheat zone and equilibrium zone
In the preheat zone, the diffusion and convection of temperature are dominant. Therefore,
the equation of the preheat temperature T
p
is
dT
p
dx
=
d
2
T
p
dx
2
. (26)
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898 A. Hmaidi et al.
The boundary conditions for the preheat zone are
x : T
p
=
T

0
T

ad
= T
0
,
dT
p
dx
= 0 (27)
x = 0 : T
p
=
T

b
T

ad
= 1
h

(28)
and, integrating Equation (26) in the preheat zone between these two boundaries gives the
solution
T
p
(x) = T
0
+
_
1
h

T
0
_
e
x
. (29)
We should note the gradient of the temperature near the reaction zone
dT
p
dx

x=0
= 1
h

T
0
. (30)
Because the fuel is not diffusive, there is no change in the fuel concentration in the preheat
zone. Only in the reaction zone, where the reaction rate becomes signicant, does the fuel
depletion sharply takes place. Hence, C
p
(x) = C
0
.
In the equilibrium zone, the fuel is totally consumed and the temperature prole is
constant, and hence we have
T
e
(x) = 1
h

, C
e
(x) = 0. (31)
3.2. Reaction zone
The reaction zone is dominated by the reaction-diffusion process, so the convection term
may be neglected. The equations for the temperature T
r
and the fuel C
r
are

d
2
T
r
dx
2
=
_
q
1
B

e
f (1
1
Tr
)
+q
2
e
(1
1
Tr
)
_
C
r
(32)

dC
r
dx
=
_
B

e
f (1
1
Tr
)
+ e
(1
1
Tr
)
_
C
r
. (33)
At the right-hand boundary of the reaction zone, near the equilibrium zone, we require
+: T
r
= 1
h

,
dT
r
d
= 0
as well as C
r
= 0,
dC
r
d
= 0
(34)
and at the left-hand boundary of the reaction, using the inner temperature expansion (16)
and the result (30), then near the preheat zone,

d
d

d
1
d

=
=
dT
p
dx

x=0
= 1
h

T
0
. (35)
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Combustion Theory and Modelling 899
3.3. Large activation energy asymptotics, 1
The framework of our approach is similar to the analysis of Matkowsky and Sivashinky
[2]. The main difference is the important addition of an endothermic reaction [3] which
represents a competitive chemical pathway. The adiabatic case treated in [2] corresponds
to h = 0 and hence can be considered as a particular case of the present system.
We combine the equations for temperature and fuel in the steady state of the reaction
zone to obtain an equation for T
r
+q
2
C
r
which we call the enthalpy equation
dT
r
dx
+q
2
dC
r
dx
=
d
2
T
r
dx
2
(q
1
+q
2
)
B

e
f (1
1
Tr
)
C
r
. (36)
This enthalpy equation is valid across all regions. For completeness therefore we have
written it as such with the convection term included. This will be used at leading order
here and, further on in this paper in Section 4.1, we will consider this at second order.
By considering this now at leading order in the reaction zone and inserting the asymptotic
expansions (16) and (17) into Equation (36), we obtain up to O(1)

_
q
2
dC
d
+
d
2

d
2
_

_
d
d

d
2

1
d
2
q
2
dC
1
d
_
= L(q
1
+q
2
)Be
f
C (37)
where L, introduced in Equation (21), is related to the eigenvalue of the adiabatic combustion
problem.
Thus, at leading order, we obtain the relationship
q
2
dC
d
+
d
2

d
2
= 0. (38)
Using the boundary conditions for the gradients at +then yields
d
d
= q
2
C, (39)
and inserting this relation in the temperature equation (32) yields, at leading order,
d
2

d
2
= Le

d
d
. (40)
By integrating this equation over the reaction zone, we obtain
_
d
d
_
=+
=
= L[e

]
=+
=
. (41)
With the boundary conditions of the reaction zone, this equation yields the following
relationship for L
L =
_
1
h

T
0
_
e
h
= (1 T
0
)e
h

he
h

. (42)
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900 A. Hmaidi et al.
Using the denition (9) and the assumption (21), the leading order result for L in Equation
(42) provides an expression for the steady burning velocity V:
V
.
=
_

c
p
e
(+h)
(1 T
0
)
A
2
. (43)
Furthermore, the asymptotic matching [6] in the enthalpy relation provides at the next order
d
d

d
2

1
d
2
q
2
dC
1
d
= L(q
1
+q
2
)Be
f
C, (44)
so that inserting the result from the rst-order matching, we obtain
d
2

1
d
2
=
_
1 +LB
q
1
+q
2
q
2
e
f
_
d
d
q
2
dC
1
d
. (45)
Asymptotic matching at the hot boundary of the reaction zone ( +) yields
d
1
d

+
=
dT
(1)
e
dx

x=f
+
(46)
T
(1)
e
(f
+
) = h (47)
C
1
0. (48)
At the cold boundary of the reaction zone ( ), we obtain
d
1
d

dT
(1)
p
dx

x=f

+
d
2
T
(0)
p
dx
2

x=f

+ (49)

T
(1)
p
(f

) +
dT
(0)
p
dx

x=f

+ (50)
C
1
0 (51)
where, in Equations (46)(51), the subscripts x = f

and x = f
+
denote just before the
ame (sited at x = 0) and just after, respectively. Using these two boundary conditions, we
integrate the previous relation and obtain for
dT
(1)
e
dx

x=f
+
+
dT
(1)
p
dx

x=f

+
d
2
T
(0)
p
dx
2

x=f

=
Le
f T
(1)
e
(f
+
)
B(q
1
+q
2
)
f q
2
+T
(1)
e
(f
+
) +T
(1)
p
(f

) +
dT
(0)
p
dx

x=f

. (52)
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Combustion Theory and Modelling 901
Regrouping the terms in this equation yields for
dT
(1)
e
dx

x=f
+
+
dT
(1)
p
dx

x=f

+
Le
f T
(1)
e
(f
+
)
B(q
1
+q
2
)
f q
2
= Z
1
Z
2
(53)
where
Z
1
T
(1)
e
(f
+
) +T
(1)
p
(f

) and Z
2

d
2
T
(0)
p
dx
2

x=f

dT
(0)
p
dx

x=f

.
In appendix A, we show that both the terms Z
1
and Z
2
are zero. Hence, we rewrite the
previous equation as
h =
Le
f h
B(q
1
+q
2
)
f q
2
. (54)
Furthermore since L
.
= (1 T
0
)e
h
, the equation for the steady-state heat loss h is
f he
h(f 1)
= (1 T
0
)
A
1
A
2
(q
1
+q
2
)
q
2
e
(1f )
. (55)
3.4. Results and discussion
From the steady-state equation for the heat loss, we identify a very important parameter
which we call . This parameter basically reects at which proportion the channelling
between endothermic and exothermic reactions takes place.
=
A
1
A
2
_
q
1
q
2
+1
_
. (56)
For the case of no heat loss it is not sufcient to simply state that q
1
= 0. As we see from
Equation (55), in order to cause the parameter to vanish we require:
h = 0 = 0 (a) A
1
= 0 or (b) Q
1
= Q
2
> 0. (57)
This means that eliminating the heat loss requires the rst reaction to be (a) either inactive
or (b) to have the same exothermicity as the second reaction.
In the expression for h in the steady state we note that the left-hand side is a strictly
monotonic increasing function of h. Hence the heat loss h is always proportional to ,
and in particular to the difference in exothermicity of both reactions, i.e. proportional to
Q
2
(Q
1
).
As these results were derived in a general framework, one could consider the pertur-
bation reaction to be either endothermic or exothermic. The results for non-dimensional
burning velocity and burnt temperature are shown in Figures 1 and 2, respectively. Gener-
ally, the conclusion is that if the exothermicity of the perturbation reaction is less than the
exothermicity of the dominant reaction, then there is a heat loss.
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Figure 1. Non-dimensional burning velocity as a function of for xed = 20 and T
0
= 0.2.
Figure 2. Non-dimensional burnt temperature as a function of f for xed = 20 and T
0
= 0.2.
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Combustion Theory and Modelling 903
An interesting consequence of this statement is that even if the perturbation reaction is
thermally neutral or even a bit less exothermic than the dominant reaction, then we should
expect a drop in the nal burnt temperature. This is due to the fact that there is competition
between these two reactions [3, 4] which means that the perturbation reaction consumes
part of the fuel that would have been consumed by the dominant exothermic reaction.
However, if the perturbation reaction has a higher exothermicity than the dominant
reaction, we expect an increase of the nal burnt temperature, i.e. h < 0 if and only if
Q
1
> Q
2
.
Remark: Due to the competitive nature of the exothermic and endothermic reactions, the
heat loss h is a derived quantity and not a direct control parameter. The control parameters
are in fact f , and . Hence, as we can see from (43), the burning velocity V is a function
of T
0
, f , and through the heat loss h.
Similar to the burning velocity, the nal burnt temperature is also a function of T
0
, f ,
and through the heat loss h.
4. Stability analysis of the travelling front
In the general case the front propagation speed is not constant in time. The reaction-
diffusion equations describing the unsteady system are given by
T
t
+
T
x
=

2
T
x
2
+
_
q
1
B

e
f (1
1
T
)
+q
2
e
(1
1
T
)
_
C (58)
C
t
+
C
x
=
_
B

e
f (1
1
T
)
+e
(1
1
T
)
_
C. (59)
4.1. Reaction zone
In the unsteady case, the enthalpy equation (the unsteady equivalent to Equation 36) is
given by
T
r
t
+q
2
C
r
t
+
T
r
x
+q
2

C
r
x
=

2
T
r
x
2
(q
1
+q
2
)
B

e
f (1
1
Tr
)
C
r
. (60)
Using a similar analysis to the steady-state analysis, we obtain the relations
q
2
C =

(61)
_

_
+

=
Le
T
(1)
e
(f
+
,t )
(t )
. (62)
The relation between C and enables us to use the jump condition of the species across the
ame to obtain an equation for :
(t )q
2
C
0
= (t )q
2
[C]
+

=
_

_
+

=
Le
T
(1)
e
(f
+
,t )
(t )
(63)
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(t )
2
=
Le
T
(1)
e
(f
+
,t )
q
2
C
0
. (64)
Taking the next order of the enthalpy equation in the reaction zone, we have
q
2
C
t

+q
2

C
1

+

2

2
= LB(q
1
+q
2
)Ce
f
(65)
and inserting (61) in (65) yields

t
_
1

+q
2

C
1

+

2

2
=
LB(q
1
+q
2
)
q
2

e
f
. (66)
It is shown in Appendix D that formal integration at second order of the enthalpy equation
(66) across the reaction zone is equivalent to the requirement that () = F() +G(t )
and hence

t
_
1

_
= 0. (67)
Hence the enthalpy result at next order (65) becomes

2
=

t
_
1

_
. ,, .
=0
+
_
+
Le
f
B(q
1
+q
2
)
q
2
_

q
2

C
1

. (68)
Asymptotic matching at the hot boundary of the reaction zone ( +) yields

+
=
T
(1)
e
x

x=f
+
(69)
T
(1)
e
(f
+
, t ) (70)
C
1
0 (71)
whereas asymptotic matching at the cold boundary of the reaction zone ( ) yields

T
(1)
p
x

x=f

2
T
(0)
p
x
2

x=f

+ (72)

T
(1)
p
(f

, t ) +
T
(0)
p
x

x=f

+ (73)
C
1
0. (74)
Remark: The fact that C
1
goes to zero at both the preheat side and the equilibrium side
suggests that the correct physical interpretation is that C
1
is zero in the reaction zone.
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Combustion Theory and Modelling 905
Using these conditions, we integrate Equation (68) and obtain for

T
(1)
e
x

x=f
+
+
T
(1)
p
x

x=f

+
Le
f T
(1)
e
(f
+
,t )
B(q
1
+q
2
)
f q
2

= Z
1
Z
2
(75)
where
Z
1
T
(1)
e
(f
+
, t ) +T
(1)
p
(f

, t ) and Z

2


2
T
(0)
p
x
2

x=f

T
(0)
p
x

x=f

.
Thus using the results in Appendix A, i.e. Z
1
, Z

2
= 0, the second-order version of the
enthalpy equation (75) then becomes
T
(1)
e
x

x=f
+
+
T
(1)
p
x

x=f

=
Le
f T
(1)
e
(f
+
,t )
B(q
1
+q
2
)
f q
2
. (76)
This important result (Equation 76) is formally derived in Appendix D. This is recast as
_
T
(1)
x
_
f
+
f

=
Le
f T
(1)
e
(f
+
,t )
B(q
1
+q
2
)
f q
2
. (77)
Recalling the result for the leading-order temperature
_
T
(0)
x
_
f
+
f

=
_

_
+

=
Le
T
(1)
e
(f
+
,t )
(t )
, (78)
it is straightforward to combine these last two results as
_
T
x
_
f
+
f

=
Le
T
(1)
e
(f
+
,t )
(t )
+
B(q
1
+q
2
)
f q
2
Le
f T
(1)
e
(f
+
,t )
(t )
. (79)
This represents the jump condition of the temperature gradient across the ame.
5. Linear stability analysis
From the asymptotic analysis [6] of the previous section we note that the jump conditions
at the ame front obtained in terms of as a parameter are now:
temperature continuity across the ame front
T
p
(f

, t ) = T
e
(f
+
, t ); (80)
jump in the temperature gradient across the ame front
_
T
x
_
f
+
f

=
Le
T
(1)
e
(f
+
,t )
(t )
+
B(q
1
+q
2
)
f q
2
Le
f T
(1)
e
(f
+
,t )
(t )
; (81)
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jump in the fuel mass fraction across the ame front

2
(t ) =
Le
T
(1)
e
(f
+
,t )
q
2
C
0
. (82)
We now proceed to analyse the reaction-diffusion equations with the above jump conditions
using a small perturbation parameter , writing
T (x, t ) = T (x) +T

(x, t ) = T (x) +

T (x)e
t
(83)
C(x, t ) = C(x) +C

(x, t ) = C(x) +

C(x)e
t
(84)
(t ) = 1 +

(t ) = 1 + e
t
. (85)
5.1. Preheat zone
In the preheat zone the temperature equation takes the form
T
p
t
+
T
p
x
=

2
T
p
x
2
. (86)
With the linear perturbation, it then becomes

p
t
+(1 +
u
)
T
p
x
+
T

p
x
=

2
T
p
x
2
+

2
T

p
x
2
. (87)
The equation for the steady terms is given by
T
p
x
=

2
T
p
x
2
. (88)
The boundary conditions of the preheat zone being
x 0 : T
p
1
h

, (89)
x : T
p
T
0
,
T
p
x
0 (90)
the expression for the preheat temperature takes the form
T
p
(x) = T
0
+
_
1
h

T
0
_
e
x
. (91)
The linearized equation for the unsteady terms is given by
T

p
t
+
u
T
p
x
+
T

p
x
=

2
T

p
x
2
. (92)
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Combustion Theory and Modelling 907
Setting r
_
+
1
4
, the solution of this equation which satises the boundary conditions
(89) is
T

p
(x, t ) = T
+
p
e
(
1
2
+r)x+t

u
_
1
h

T
0
_
e
x+t
. (93)
5.2. Equilibrium zone
In the equilibrium zone, the temperature is governed by the following equation
T
e
t
+
T
e
x
=

2
T
e
x
2
. (94)
With the linear perturbation approach, this equation takes the form

e
t
+(1 +
u
)
T
e
x
+
T

e
x
=

2
T
e
x
2
+

2
T

e
x
2
. (95)
The steady term obeys the following equation
T
e
x
=

2
T
e
x
2
. (96)
The boundary conditions of the equilibrium zone are
x +: T
e
1
h

,
T
e
x
0 (97)
and hence the stationary temperature in the equilibrium zone is
T
e
(x) = 1
h

. (98)
Since T
e
is constant,the equation for the unsteady term T

e
is given by
T

e
t
+
T

e
x
=

2
T

e
x
2
. (99)
The solution of this equation, which satises the boundary conditions (97), is then
T

e
(x, t ) = T

e
e
(
1
2
r)x+t
. (100)
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5.3. Derivation of frequency condition
We apply the continuity condition (80) and jump conditions (81) and (82) to the unsteady
solutions of the preheat and postame temperatures. This yields a solvability condition
which is given by
4r
3
(Le
h
+(1 2f )h)r
2
+(Le
h
h 1)r
1
4
(Le
h
+(3 2f )h) = 0.
(101)
As in [2] we use as bifurcation parameter a number , which is half the Zeldovich number [5],
and it is dened as

Le
h
2
.
=
(1 T
0
)
2
(102)
so that the frequency equation can be written as
4
2

_ _
h
_
f
1
2
__
2
4
_

h
2
_
1
_
+(h(f 1) +1)
_

h
2
_
= 0.
(103)
The solutions of the frequency equation are

=
_
h
_
f
1
2
__
2
4
_

h
2
_
1
8
(104)

1 h
_
f
1
2
_

8
_

2
2
_
3+h
_
f
1
2
__
+
_
h
_
f
1
2
_
1
_
2
+4h.
Note that, in the adiabatic case, the special case corresponding to h = 0, these results
collapse to those obtained in [2]:
4
2

2
4 1
_
+ = 0. (105)
The solutions of the frequency equation in the adiabatic case are
=

2
4 1 | 1|

2
6 +1
8
.
In the general case the equation for the neutral stability ((w) = 0) is given by
_

h
2
_
_

2
2
_
2 +h
_
f
1
2
__
+h
2
_
f
1
2
_
2
+2h 1
_
= 0. (106)
In Figure 3 the complex eigenfrequencies
+
() and

() start for = 0 at two

different locations with a zero imaginary part. These are marked by for the h = 0.5 case.
As increases, the real parts merge at point A, where 0.2859, and then move in the
complex plane with a negative real part until 5.3958. At this value of corresponding
to B
1
and B
2
, the real part of the eigenfrequencies becomes positive.
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Combustion Theory and Modelling 909
Figure 3. Imaginary part vs. real part of eigenfrequency as a function of for h = 0 and h = 0.5
with f = 2.
Figure 4. Non-dimensional heat loss parameter h as a function of for f = 2 and T
0
= 0.33. As
dened in Equation (102), is related to the reduced activation energy and represents half the
Zeldovich number.
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5.4. Critical values of for a given h
5.4.1. Stability domain
The solutions to the neutral stability equation are

o
st
(h) =
h
2
or

st
(h) = 2 +h
_
f
1
2
_

_
5 +4h(f 1). (107)
The condition of stability of the unsteady terms ((w) 0) is satised whenever
max
_

o
st
(h),

st
(h)
_

+
st
(h). (108)
The lower bound for is
max
_

o
st
(h),

st
(h)
_
=
_

o
st
if h(f 1) 1

st
if h(f 1) > 1.
(109)
5.4.2. Oscillation domain
To obtain the oscillation domain, we need to determine the values of for which the values
of
+
and

collapse. Requiring that

+
=

, i.e. r
+
= r

, leads to three values of :

osc
(h)=3 +h
_
f
1
2
_
2
_
2 +2h(f 1) or
o
osc
(h)=1 +h
_
f
1
2
_
. (110)
Only

osc
are interesting, since
o
osc
corresponds to
+
=

with () = 0. Hence, the

system is oscillatory for all values of in the range [

osc
,
+
osc
].
Furthermore, we require the non-dimensional nal temperature 1 h/ to be
larger than the initial temperature T
0
. Therefore, we restrict to the half-plane where
h/2 > 0.
5.5. Critical values of h for a given
5.5.1. Stability domain
The solutions to the neutral stability equation are
h
o
st
() = 2 or h

st
() =
_
f
1
2
_
1
_
_
f
1
2
_
2
(4 +1) 2
_
f
1
2
_
+1
_
f
1
2
_
2
.
(111)
The condition of stability of the unsteady terms ((w) 0) is satised whenever
max
_
h
o
st
(), h

st
()
_
h h
+
st
(). (112)
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Combustion Theory and Modelling 911
The lower bound for is
max
_
h
o
st
(), h

st
()
_
=
_
h
o
st
if 2(f 1) 1
h

st
if 2(f 1) > 1.
(113)
5.5.2. Oscillation domain
To determine the oscillation domain, we need the values of h for which the two solutions
of collapse. Requiring that
+
=

, i.e. r
+
= r

, leads to
h
o
osc
() =
1
f
1
2
or
h

osc
() =
1
f
1
2
+
2
_
f
3
2
_
2
_
2(f 1)
_
f
1
2
_

_
f
3
2
_
_
f
1
2
_
2
. (114)
5.6. Results and interpretation
In Figure 4 we identify the regions of stability and oscillation in the h- space for different
values of .
From this gure we note that for a given h < 1/(f 1) there is for low values of
a region of non-oscillatory unstable behaviour, which as increases tracks regions that
are (in order) non-oscillatory stable, oscillatory stable, non-oscillatory stable and then
non-oscillatory unstable again. However, if h > 1/(f 1), the two rst regions are non-
oscillatory unstable and then oscillatory unstable.
Figure 4 also shows a wide region of stable oscillatory behaviour in the h- diagram.
However, is typically greater than 4 and h is likely to be small in these problems, so that
it becomes evident that the oscillatory unstable region is easily reached.
Shown also are heat loss curves from the steady-state analysis indicating stationary
results for different values of . It is important to note that a steady state with given
activation energies ( and f values) and a given endothermic channel ( value) will
then be represented by a single point on the h- diagram of Figure 4. Consequently, for
most practical condensed phase combustion wave problems where a small competitive
endothermic reaction is present, the steady-state solution can easily lie in the band of
oscillatory stability and there is likely to be an unsteady front propagation.
Numerical simulations of the front propagation obtained by integrating Equations (1)
and (2) are consistent with the analytical results. In fact, a numerical simulation of the case
= 5 and = 0, corresponding to the adiabatic case, shows in Figure 5 the oscillatory in-
stability that Matkowsky and Sivashinsky demonstrated theoretically in [2]. As we increase
the value of to move to the case of heat loss through a competitive endothermic reaction,
we obtain for = 5 and = 10
4
an unsteady ame propagation as can be seen in Figure
6. Furthermore, as we should expect from the analytical results for = 5 and = 5 10
5
,
the numerical simulation in Figure 7 shows a steady propagation of the temperature prole
without oscillation.
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Figure 5. Temperature prole at different time steps for = 5, = 0 and f = 2. This corresponds
to the adiabatic case.
Figure 6. Temperature prole at different time steps for = 5, = 10
4
and f = 2.
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Combustion Theory and Modelling 913
Figure 7. Temperature prole at different time steps for = 5, = 5 10
5
and f = 2.
6. Conclusions
In this paper we have proposed a mathematical model of the stability of a combustion front
propagating through a solid fuel, in the case where, in addition to the leading exothermic
reaction, there is also a competitive endothermic reaction. Treating the endothermic re-
action as a perturbation to the leading order exothermic reaction, and assuming that the
endothermic reaction activation energy is larger than that of the exothermic reaction, we
have used large activation energy asymptotic methods to derive the heat loss, and conse-
quently the ame temperature and the burning velocity. Matkowsky and Sivashinsky [2]
showed that there is a region in parameter space exhibiting oscillatory unstable behaviour
for > 2 +

5. In our case the extra effect of the endothermic competitive reaction is to

shift the region of oscillatory unstable behaviour in parameter space towards higher values
of and thus higher values of the activation energy.
This paper shows that many practical solid phase combustion waves are likely to be
unstable to linear disturbances. Numerical simulations suggest nite amplitude oscillations
in front propagation as in Figures 5 and 6, which should be amenable to prediction by a
nonlinear stability analysis beyond the scope of the present work. The numerical results
indicate that there will be nite amplitude response in the nonlinear oscillations.
References
[1] J. Buckmaster, The quenching of deagration waves, Combust. Flame 26 (1976), pp. 151162.
[2] B. Matkowsky and G. Sivashinsky, Propagation of a pulsating reaction front in solid fuel
combustion, SIAM J. Appl. Math. 35 (1978), pp. 465478.
[3] P. Simon, S. Kalliadasis, J. Merkin, and S. Scott, Inhibition of ame propagation by an en-
dothermic reaction, IMA J. Appl. Math. 68 (2003), pp. 537562.
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914 A. Hmaidi et al.
[4] R. Ball, A. McIntosh, and J. Brindley, Thermokinetic models for simultaneous reactions: A
comparative study, Combust. Theory Model. 3 (1999), pp. 447468.
[5] J. Buckmaster and G. Ludford, Theory of Laminar Flames, Cambridge University Press, Cam-
bridge, 1982.
[6] W. Bush and F. Fendell, Asymptotic analysis of laminar ame propagation for general Lewis
numbers, Combust. Sci. Technol. 1 (1970), pp. 421428.
Appendix A
For term Z
1
The temperature is continuous across the ame front:
T
(0)
p
(f

, t ) +
1

T
(1)
p
(f

, t ) = T
p
(f

, t ) = T
e
(f
+
, t ) = T
(0)
e
(f
+
, t )
1

T
(1)
e
(f
+
, t ).
(1)
Hence we have
Z
1
T
(1)
p
(f

, t ) +T
(1)
e
(f
+
, t ) = 0. (2)
For terms Z
2
and Z

2
We note that for = 1 we have Z
2
= Z

2
. Hence we will consider the general case for .
In the preheat zone the temperature equation takes the form
T
p
t
+
T
p
x
=

2
T
p
x
2
. (3)
As the preheat temperature is written as
T
p
(x, t ) = T
(0)
p
(x, t ) +
1

T
(1)
p
(x, t ) + (4)
we have at leading order
T
(0)
p
t
+
T
(0)
p
x
=

2
T
(0)
p
x
2
(5)
which is equivalent to
T
(0)
p
t
=

2
T
(0)
p
x
2

T
(0)
p
x
(6)
and means that
Z

2


2
T
(0)
p
x
2

x=f

T
(0)
p
x

x=f

=
T
(0)
p
(f

, t )
t
= 0. (7)
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Combustion Theory and Modelling 915
Appendix B
Heat loss equation in steady state
By combining the steady form of Equations (58) and (59) we may eliminate the dominant
reaction term and obtain
dT
dx

d
2
T
dx
2
+q
2
dC
dx
= (q
1
+q
2
)
B

e
f
C. (1)
Integrating this relation over the whole domain, we obtain
[T q
2
C]
x=+
x=
= (q
1
+q
2
)
B

_
=+
=
e
f
Cd. (2)
If the boundary conditions for T are given by
x : T = T
0
, C = C
0
(3)
x +: T = 1
h

, C = 0 (4)
at leading order we have that
1 T
0
= q
2
C
0
. (5)
For the rst-order terms the integral relation is equivalent to
h = L(q
1
+q
2
)B
_
=+
=
e
f
Cd. (6)
Since q
2
Cd = d, we obtain that
h = L
_
q
1
q
2
+1
_
B
_
e
f
f
_
=h
=+
(7)
which yields the relationship
f he
f h
= L
_
q
1
q
2
+1
_
B. (8)
Due to the relation
L =
_
1
h

T
0
_
e
h
.
= (1 T
0
)e
h
(9)
the equation for the heat loss takes the form
f he
(f 1)h
= (1 T
0
)
_
q
1
q
2
+1
_
B. (10)
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916 A. Hmaidi et al.
For the limiting case f = 1, we obtain
h = (1 T
0
)
A
1
A
2
_
q
1
q
2
+1
_
. (11)
Appendix C
Solving the PDE for the unsteady preheat temperature
At rst-order in we obtain the equation for the unsteady term
T

p
t
+
u
T
p
x
+
T

p
x
=

2
T

p
x
2
. (1)
Inserting the ansatz for the unsteady terms in this equation, we get

T
p
+


T
p
x

2

T
p
x
2
=
u
T
p
x
. (2)
The solution to the homogeneous version of this equation is

T
o
p
(x) = T
+
p
e
(
1
2
+r)x
+T

p
e
(
1
2
r)x
(3)
where r is dened as r =

+
1
4
. Note that (r)
1
2
.
To obtain the solution of the non-homogeneous equation we add the particular solution
s =
u
T
p
x
and obtain

T
p
(x) =

T
o
p
(x)
u
T
p
x
= T
+
p
e
(
1
2
+r)x
+T

p
e
(
1
2
r)x

u
_
1
h

T
0
_
. (4)
Since the unsteady terms vanish as x , we require T

p
= 0 and we have

T
p
(x) = T
+
p
e
(
1
2
+r)x

u
_
1
h

T
0
_
e
x
. (5)
Appendix D
Concerning the integration of Equation (66)
The inner Equation (66) of the main text represents the enthalpy condition across the
reaction zone. It is given by

t
_
1

+q
2

C
1

+

2

2
=
LB(q
1
+q
2
)
q
2

e
f
. (1)
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Combustion Theory and Modelling 917
Integrating this equation across the inner zone gives

t
_
1

T
(1)
ef
[ ]

T
(1)
ef
+q
2
[ C
1
]

T
(1)
ef
+[ C
1
]

T
(1)
ef
+[

1

T
(1)
ef
=
LB(q
1
+q
2
)
q
2
_

T
(1)
ef
e
f
d (2)
where
T
(1)
ef
T
(1)
e
(f
+
, t )
and note that as , , and as , T
(1)
ef
.
Thus Equation (D2) can be written as,

t
_

+

t
[
T
(1)
ef

] |

+ T
(1)
ef
+ q
2
C
1
|

q
2
C
1
|
T
(1)
ef
+

1

T
(1)
ef
=
LB(q
1
+q
2
)
f q
2
[ e
f
]

T
(1)
ef
.(3)
From matching (main text, Equations 46, 48 and 49) we have

=
T
(1)
p
x

x=f

2
T
(0)
p
x
2

x=f

|
T
(1)
ef
= 0

T
(1)
ef
=
T
(1)
e
x

x=f
+
.
Hence Equation (D3) becomes

t
_

+

t
_
T
(1)
ef

_
|

+ T
(1)
ef
+ q
2
C
1
|

T
(1)
p
x

x=f

2
T
(0)
p
x
2

x=f

T
(1)
e
x

x=f
+
=
LB(q
1
+q
2
)e
f T
(1)
ef
f q
2
. (4)
The leading order matching condition for gradients on the preheat side is

=
T
(0)
p
x

x=f

. (5)
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918 A. Hmaidi et al.
Hence
|

T
(0)
p
x

x=f

T
(1)
p

x=f

. (6)
Consequently Equation (D4) can be written as

t
_
T
(1)
ef

_
+ T
(1)
ef

T
(1)
p
x

x=f

+
T
(1)
p

x=f

T
(0)
p
x

x=f

2
T
(0)
p
x
2

x=f

T
(1)
e
x

x=f
+
+ q
2
C
1
|

t
_

+
|

T
(0)
p
x

x=f

2
T
p
(0)
x
2

x=f

=
LB(q
1
+q
2
)e
f T
(1)
ef
f q
2
. (7)
It is therefore necessary to have both non-growing and growing terms in Equation (D7) to
balance.
Firstly the growing terms of Equation (D7) require that
D(t ) + q
2
C
1
|

t
_

_
+

T
(0)
p
x

x=f

_

T
(0)
p
x

x=f

2
T
(0)
p
x
2

x=f

_
. (8)
The last bracketed term in Equation (D8) is zero because of the form of the preheat
equation (see Equation 86 in the main text) and the function D(t ) is to be determined from
the non-growing terms in Equation (D7).
Consider now the second term on the right-hand side of Equation (D8). From Equation
(61) in the main text, matching on the preheat side at leading order gives
T
(0)
p
x

x=f

= q
2
C
0
. (9)
But from Equation (7) in the main text
T

ad
T

0
=
Q
2
C
0
c
p
.
Hence using the denition (11c) in the main text we have
1 T
0
= q
2
C
0
so that Equation (D9) becomes
T
(0)
p
x

x=f

= (1 T
0
) . (10)
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Combustion Theory and Modelling 919
Consequently Equation (D6) becomes
|

(1 T
0
) T
(1)
p

x=f

so that
_

(1 T
0
)
1

T
(1)
p

x=f

and thus
_

t
_
T
(1)
p

_
. (11)
We can now see that the condition for the growing terms (D7) is now
q
2
C
1
|

D(t ) +

t
_
T
(1)
p

_
. (12)
Secondly consider the non-growing terms of Equation (D7). These require that
D(t ) +

t
_
T
(1)
ef

_
+ T
(1)
ef
+
T
(1)
p

x=f

T
(0)
p
x

x=f

2
T
(0)
p
x
2

x=f

T
(1)
p
x

x=f

T
(1)
e
x

x=f
+
=
LB(q
1
+q
2
)e
f T
(1)
ef
f q
2
. (13)
where note that again the function D(t ) is included since we included a D(t ) in the
growing terms condition (D8) of Equation (D7).
Because T
(1)
p

x=f

= T
(1)
ef
and noting again the form of the preheat equation (see
Equation 86 in the main text), the third and fourth terms cancel in Equation (D13) so that
Equation (D13) becomes
D(t ) +

t
_
T
(1)
ef

_

T
(1)
p
x

x=f

T
(1)
e
x

x=f
+
=
LB(q
1
+q
2
)e
f T
(1)
ef
f q
2
. (14)
This indicates that the natural choice for D(t ) is
D(t ) =

t
_
T
(1)
ef

_
(15)
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920 A. Hmaidi et al.
and we thus have the second-order condition on gradients
T
(1)
p
x

x=f

+
T
(1)
e
x

x=f
+
=
LB(q
1
+q
2
)e
f T
(1)
ef
f q
2
(16)
which is Equation (76) in the main text.
Note that this is equivalent to (before inner integration), setting
(1 T
0
) T
(1)
ef
(17)
so that

t
(
1

) = 0 right from the outset in Equation (D1). This is consistent with the
statement () = F() +G(t ) after Equation (66) in the main text.
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