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Article history: The ame propagation in a solid composite energetic sample comprised of a solid energetic annulus
Received 20 December 2016 surrounding a highly conductive core is investigated using one-step Arrhenius reaction mechanism. The
Revised 7 March 2017
steady-state solutions, its linear stability analysis and the results of direct numerical simulations of non-
Accepted 14 April 2017
stationary problem are presented. It was found that the ame dynamics is highly subject to variation in
the presence of the conductive core leading in some cases to a chaotic ame behavior or to stabiliza-
Keywords: tion of the ame propagation. It was demonstrated that for given combustion properties of the energetic
Combustion waves material the kind of ame dynamics observed in the composite sample can be controlled by an appro-
Thermal-diffusive instabilities priate choice of the experimental parameters such as the thickness of the fuel annulus deposited or the
Composite energetic materials
diameter of the heat conductive core.
Flame oscillations
2017 The Combustion Institute. Published by Elsevier Inc. All rights reserved.
1. Introduction asymptotic analysis [10]. It was demonstrated that the planar com-
bustion wave loses stability due to the Hopf bifurcation and the
The onset of pulsations quite often accompanies the propaga- critical parameter values for the onset of oscillations and character-
tion of combustion waves in solid combustion fuels. One of the istics of these oscillating regimes were determined. These ndings
rst experimental observation was reported in [1]. In the lat- were later conrmed in numerical analysis in [11,12].
ter experimental papers [2,3] it was demonstrated that pulsations In the case of the cylindrical geometry it was shown [13] that
are of auto-oscillatory nature and that complex temporal regimes as the diameter of the sample is increased either traveling or one-
can emerge as the bifurcation parameters (mixture dilution) are dimensional pulsating instabilities occur, which can result in the
modied. Besides planar one-dimensional oscillations in cylindri- emergence of spinning or pulsating regimes of combustion wave
cal solid fuel samples multidimensional regimes of ame propaga- propagation. The results of the stability and bifurcation asymptotic
tion such as spinning waves were found while conducting the self- analysis in the limit of the large activation energy are summarized
propagating high temperature synthesis [4,5]. More detailed de- in [14]. Extensive numerical results of combustion wave propa-
scription of the variety of spatio-temporal wave patterns observed gation in cylindrical samples were presented in [1519] where
in combustion of solid fuels can be found in reviews [68]. the emergence of different nonstationary and/or multidimensional
Systematic mathematical analysis of oscillatory ame propaga- regimes of ame propagation was reported. In [20] the numeri-
tion regimes began with the publication of the results in [9], where cal stability analysis of combustion wave propagation in cylindrical
it was demonstrated by means of numerical modeling that the pla- fuel sample was undertaken and the formation of different modes
nar ame pulsations are of diffusional-thermal nature and can be of spinning waves was directly related with the global stability
described within the models which take into consideration heat characteristics of two-dimensional traveling wave solutions.
release occurring in course of fuel consumption and heat diffu- Initiated by the works in [21,22] the idea to develop the solid
sion from hot products to the fresh mixture. Further advances in nanostructured composite energetic materials is actively discussed.
the analysis of ame pulsations came from the employment of the These materials structurally are comprised of the solid fuel shell
which provides the heat due to the chemical reaction and in-
ert core with high thermal conductivity, which serves as a ther-
Corresponding author. mal conduit to recuperate heat from hot products of the reac-
E-mail address: vadim.k@ciemat.es (V.N. Kurdyumov). tion to the fresh fuel mixture. The core can be made of carbon
http://dx.doi.org/10.1016/j.combustame.2017.04.019
0010-2180/ 2017 The Combustion Institute. Published by Elsevier Inc. All rights reserved.
168 V.N. Kurdyumov et al. / Combustion and Flame 182 (2017) 167178
The parameters appearing in the above equations are Appropriate boundary conditions corresponding the congura-
tion depicted in Fig. 1 are
KP exp(E/RTa ) 2 1 c 1 S 1
= , = , s= , (9) x : 1 = 2 = Y 1 = 0 ,
1 c 1 S 1 B 1 2 c 2 S 2 (14)
x + : Y/ x = 1 / x = 2 / x = 0.
where 1 = 1 /1 c1 and 2 = 2 /2 c2 are the thermal diffusivi-
Finally, the problem of the ame propagation in the composite en-
ties. It is noteworthy that the parameter s can be easily changed
ergetic sample is reduced to solve Eqs. (6)(7) and (11) subject to
in experiments by varying the cross-section of the conductive core
the boundary conditions given by Eq. (14).
or deposited mass of the energetic material in the annulus. In
the limit 0 Eqs. (6)(7) become identical to those describing
3. Numerical treatment
a standard one-dimensional combustion wave propagating in the
pure energetic sample [9].
Steady as well as time-dependent computations were carries
In the following we assume that that the cross-section of the
out in a nite domains, xmin < x < xmax . The typical values were
conductive core is small compared with that of the solid com-
xmin = 20 and xmax = 20. The spatial derivatives were discretized
bustible, S2 S1 , and, simultaneously, it has a very high thermal
on a uniform grid using second order three-point central differ-
conductivity compared with that of the energetic annulus, namely
ences for the temperature in Eq. (7) and three-point upwind dif-
2 1 . In term of the non-dimensional parameters it means that
ferences for the convection term of Eq. (6). The typical number
s 1 and 1. It is convenient to introduce a parameter de-
of grid points was 2001. For time-dependent computations an ex-
ned as
plicit marching procedure was used in time with the typical time
2 S2 step = 104 . The number of grid points was doubled in some
= = . (10)
cases and was halved without any signicant differences in the
s 1 S1
results. In order to determine steady solutions (but not necessary
Always supposing that = O(1 ), Eq. (8) takes in the limit s stable), the steady counterpart ( / t 0) of Eqs. (6)(7) were
the following quasi-steady form solved together with Eq. (11) using a GaussSeidel method with
2 2 over-relaxation.
0= + ( 1 2 ) . (11)
x2 4. Steady-state solutions
This approximation describes conductive cores of negligible heat
capacity with non-negligible heat transfer effect. This situation cor- Consider rst the steadily propagating ames imposing / t =
responds to an experimental setup where the single carbon nan- 0 in Eqs. (6), (7) which were solved together with Eqs. (11) and
otube form the heat conducting core of the composite material (14). The system has the rst integral,
[22].
d 1 d 2
The dimensionless reaction rate appearing in Eqs. (6)(7) is u f ( 1 + Y 1 ) = + , (15)
dx dx
given by
indicating, together with Eq. (11), that 1 1 and 2 1 behind
( 1 )
the ame where the fuel mass fraction and temperature gradients
= Y exp 1
(12)
1 + ( 1 1 ) approach to zero value.
Figure 2 illustrates the typical distributions of the mass fraction
The factor appearing in Eq. (12) provides that uf 1 for the
and temperatures plotted for = 5, = 5, = 8 and = 0.7. The
steady combustion wave in the pure energetic material in the limit
distinctive characteristic of the temperature prole in the energetic
. material is the existence of a local maximum appearing just after
The instantaneous values of u f (t ) = tcU f /lc are determined by
the reaction zone with the super-adiabatic temperature, 1 max > 1.
the additional condition
The dimensionless steady velocity uf is shown in Fig. 3 (left
1 ( x , t ) = , (13) plot) together with the temperature maximum, 1 max (right plot),
as functions of for various , all curves calculated for = 8 and
where = (T T0 )/(Ta T0 ) is the non-dimensional reference = 0.7. It can be seen in Fig. 3 that the temperature in the an-
temperature. Evidently, all results should be independent on x nulus can be more than 30% higher than the adiabatic ame tem-
due to translation invariance along the direction of motion, x perature in pure solid fuel, while the ame speed can increase in
x + const. more than ve times. The gure shows also that for small values
1
8
1
6
Y 2 4
0.5
0
-20 -15 -10 -5 0 5 x 10
0
Fig. 2. Typical steady mass fraction and temperatures proles computed using the reduced model given by Eqs. (7), (6) and (11).
170 V.N. Kurdyumov et al. / Combustion and Flame 182 (2017) 167178
=5
4
=5 =10
1.2 =1
=1
3
=0.1
1.1
2
=0.1
1
1
0 5 10 15 0 5 10 15
Fig. 3. Computed steady ame velocity uf (left) and maximum of the temperature 1 (right) as a function of ; for = 8, = 0.7 and several values of .
of the maximum temperature 1 max approaches to unity and are both functions of x. The constraint following from Eq. (13) be-
the ame velocity becomes uf 1.02 calculated for = 8, = 0.7 comes
and = 0. It can be explained by the fact that the effect of the
conductive core becomes negligible not only for 0, as it was 1 (x ) = 0 (20)
mentioned above, but also for 0 when 1 2 . The solution of Eqs. (1719) is sought in the form
Stability analysis of the steady-state ames presented in the where ( h , 1h , 2h ) is the solution of homogeneous system ob-
previous section has been carried out using the method described tained from Eqs. (1719) by imposing u f 1 = 0 and c is a constant.
in detail in [29]. The distributions of the steady-state temperatures, The values of uf1 and c can be found by substituting (21) into
mass fraction and the ame propagation velocity, all now denoted Eqs. (17)(19) and (20). It leads to
by subindex 0, are perturbed as usual with small perturbations
c = {1h /0I }|x=x , u f 1 = c.
i = i0 (x ) +
i (x ) exp(t ), i = 1, 2, Finally, the eigenvalue can be calculated by solving the homoge-
Y = Y0 (x ) +
(x ) exp(t ), (16) neous counterpart (imposing u f 1 = 0) of Eqs. (17)(19) with con-
straint (20) omitted without loss of generality. In what follows
u f = u f 0 +
u f 1 exp(t ),
subindex h denoting the homogeneous solution will not be ap-
plied.
where is a complex number, the real part of which represents of
It should be noted that the steady-state solutions in the
the growth rate, and
is a small amplitude. The linearized eigen-
form of traveling waves are always invariant with respect to a
value problem obtained when substituting Eqs. (16) into Eqs. (6),
shift x x + const. It leads to existence of the eigenvalue =
(7) and (11) reduces to nd non-trivial solutions of the system
0 with the corresponding eigenfunction given by ( , 1 , 2 ) =
+ u f 1Y0I + u f 0 I = A1 B , (17) (dY0 /dx, d10 /dx, d20 /dx ). The method applied in this study is
able to calculate the eigenvalue with the largest real part, see [29].
Then, the eigenvalue = 0 can be obtained as a result (within nu-
1 + u f 1 0I + u f 0 I1 = II1 + A1 + B (1 2 ), (18) merical accuracy) in the case of a stable combustion wave.
=0.8 0.8
0.2
0.3 0.1
0.6 0
=0.7 =5
0 0.5 1 1.5
0.2
=1
0.4
0.1
=0.1
=0.6 0.2
0
6.5 7 7.5
8
R I
=4
=3
0.03 =5 1.5
=5
0.02 1
=4
0.01 0.5
=3
0
0
0 0.5 1 1.5 2 2.5 0 0.5 1 1.5 2 2.5
Fig. 5. The growth rate R (left) the frequency of oscillation I (right) as a function of calculated for = 7.2, = 0.7 and various . The critical values of are indicated
with open circles; open triangles in the left gure indicate the numerical cases shown in Fig. 7 for = 5; open diamond symbols in both gures show the growth rate and
the frequency of oscillations computed from the time-dependent numerical simulations for = 5 and various .
172 V.N. Kurdyumov et al. / Combustion and Flame 182 (2017) 167178
1.4 =0.1
uf
1.2
t
0.8
0 100 200 300 400
2 =1
uf
1.5
t
1
0 50 100 150 200
3
=2.5
uf
t
1
0 50 100 150 200
Fig. 7. Time histories of the ame velocity calculated for = 7.2, = 0.7, = 5 and several values of corresponding open triangles in Fig. 5; the reference temperature
is xed at = 0.5 for all cases.
be negative. The critical values of above which the ame propa- to a time-periodic state, with the ame velocity uf oscillating with
gation becomes stable (R < 0) are marked with open circles. constant frequency and amplitude. Thus, for relatively low the
ame propagation remains stable as well as in the pure energetic
7. Unsteady ame dynamics sample. It becomes unstable undergoing periodic oscillations when
is increased above the rst critical value , but a further in-
In the present section the results of the linear stability analy- crease in above the second critical value leads eventually to
sis are contrasted with the nonlinear ame dynamics. The time- re-stabilization of the ame propagation.
dependent problem given by Eqs. (67) and (11) was solved nu- The time-dependent numerical simulations themselves can be
merically. Consider rst the case = 7.2 for which the combus- used to evaluate the ame stability properties, see [30]. We show
tion wave is stable (the ame velocity is a constant in time) in in Figs. 5 and 6 with open diamond symbols the growth rate R
the pure energetic sample. Figure 7 shows the time-histories of and the frequency of oscillations I based on Eqs. (6)(7) and
uf calculated for = 5 and three values of marked with trian- (11) computed for = 5 and various . One can see a good t of
gles in Fig. 5. This plot demonstrates that for = 0.1 and = 2.5 these results to the linear stability analysis.
the ame approaches after a transient stage of behavior a stable The ame dynamics becomes much more complex for higher
steady state. For = 1, on the other hand, the solution evolves values of the Zeldovich number. Consider the case = 8 and =
V.N. Kurdyumov et al. / Combustion and Flame 182 (2017) 167178 173
6
6
=1
5 =0.1 5
4
4
3
3
2
2
1
1
0
0 0 20 40 60 80 100 120 140 160 180 200
0 20 40 60 80 100 120 140 160 180 200
6 =2.2 6 =2.5
5 5
4 4
3 3
2 2
1 1
0 0
0 20 40 60 80 100 120 140 160 180 200 0 20 40 60 80 100 120 140 160 180 200
6
=3 6
=3.5
uf uf
4 4
2 2
0
0 50 100 150 t 200 0
0 50 100 150 t 200
6
=4.0 6
=5.0
uf uf
4 4
2 2
0
0 50 100 150 t 200
0
0 10 20 30 40 t 50
Fig. 8. Time histories of the ame velocity calculated for = 8, = 0.7, = 5 and several values of ; the reference temperature is xed at = 0.5 for all cases.
0.7 when the combustion wave is already unstable in the pure en- Despite the local in time chaotic behavior of uf revealed in
ergetic sample. In Fig. 8 we show the time-history of uf for vari- some cases, the time-average ame velocity is always a constant.
ous values of . All cases were calculated for = 5 and the refer- Let us introduce the value
ence temperature was xed at = 0.5. One can see that with in-
creasing values of the ame dynamics suffers important changes 1 t
u f = u f (t )d t . (22)
evolving from merely oscillatory, as shown by the = 0.1 case, t 0
through the period-doubling route, the cases = 1 and 2.2, to the
chaotic behavior illustrated with = 2.5 and = 3. It is notable In fact, Eq. (22) represents the mean travel distance per unit time.
that further increase in produces the inverse period doubling The limiting value of u f calculated at t gives the time-average
cascade illustrated with the = 4 case, and, nally, leads to stabi- ame velocity. Shown in Fig. 10 is the time history of u f calcu-
lization of the ame propagation shown for = 5. lated for = 8, = 5 and = 3. The solid line and points in this
The chaotic ame dynamics found for = 3 is compared with gure show the cases calculated for = 0.5 and = 0.8, respec-
the simple oscillatory behavior observed for = 0.1 in Fig. 9 tively. One can see that the limiting value of u f is independent on
where the dependence of the temperature maximum 1 max is plot- the choice of used to attach the reference frame to the ame,
ted versus the ame velocity uf . as it should be. It means that the ame as a whole propagates as
174 V.N. Kurdyumov et al. / Combustion and Flame 182 (2017) 167178
1.5 1.5 =3
1 max =0.1 1 max
1.4 1.4
1.3 1.3
1.2 1.2
1.1 1.1
1 1
0 1 2 3 4 uf 5 0 1 2 3 4 uf 5
Fig. 9. The dependence of 1max versus uf for the mere oscillatory dynamics (left plot) and the chaotic regime (right plot).
_3 =8, =5, =3
uf the steady flame velocity
2.5
2
the time-avarage flame velocity
1.5
1
0 200 400 600 800
t 1000
Fig. 10. Time history of u f dened by Eq. (22) calculated for = 8, = 5 and = 3; the cases computed with = 0.5 and 0.8 are shown with a solid line and points,
respectively. The steady ame velocity is indicated with a dashed line.
a compact structure with a constant time-average ame velocity inverse doubling cascade are observed, as shown for = 3.5, 3.7
while its parts suffer the local chaotic motion in time around mean and 4.
values. It is interesting also that this time-average velocity results
smaller than the velocity of the corresponding (unstable) traveling 8. Lyapunov characteristic exponent
wave solution reported in Section 4 and shown in Fig. 10 with a
dashed line. Evidently, the ame dynamics considered as a whole should
The simplest tool to illustrate variations in the ame dynamics be independent on the reference frame used to describe the pro-
is the rst return map technics. Using the dependence of uf as a cess. In the present study we use the reference frame attached to
function of time the series of the local maximum of the ame ve- a point with a xed temperature, = . For the steady propaga-
locity are identied, {u f n , n = 1, 2, . . . }, where n is the maximum tion the ame moves as a rigid structure and the (constant) ame
number. The dependence of u f (n+1 ) versus uf n is plotted in Fig. 11 velocity uf is independent on due to invariance with respect to
for various . These pictures display the evolution of the ame dy- a shift along the direction of motion, x x + const. In the case of
namics with increasing values of . unsteady ame dynamics the ame does not move as a rigid struc-
The case = 0.1 illustrates a simple oscillatory behavior with ture, because each point of the ame moves with own velocity.
the only maximum of uf during the period: the rst return map Consequently, the specic form of uf does depend on the choice of
consists of a single point. The rst return maps for = 1 and the reference temperature . In a certain sense the specic value
= 2.2 contain two and four points, respectively, indicating the of plays the role of an observable parameter determined by the
typical period doubling cascade. The further increase in pro- choice an experimentalist.
duces the rst return map to be continuous evidencing the chaotic Figure 12 shows the rst return maps calculated for the same
behavior of uf on time. It is interesting to see in Fig. 11 that for set of the physical parameters and different values of the reference
= 2.5 the rst return map consists of various separated contin- temperature in the case of the chaotic ame dynamics. The g-
uous parts which merge later for higher values of , as shown for ure shows that the maps are qualitatively similar, as one would
= 3. Thereafter, with further increase of , the rst return map expect, but the amplitude of chaotic oscillations is affected signi-
is split again into various parts, as shown for = 3.42. Finally, the cantly by the choice of .
V.N. Kurdyumov et al. / Combustion and Flame 182 (2017) 167178 175
6 6
=0.1 =1
uf(n+1) uf(n+1)
5 5
4 4
3 3
2 2
2 3 4 5 ufn 6 2 3 4 5 ufn 6
6 6
=2.2 =2.5
uf(n+1) uf(n+1)
5 5
4 4
3 3
2 2
2 3 4 5 ufn 6 2 3 4 5
ufn 6
Fig. 11. The rst return maps of the relative maximum of uf plotted for = 8, = 0.7, = 5 and various .
The level of randomness of time series can be characterized by shell-inert core type is derived and investigated for practically im-
the Lyapunov characteristic exponent [31]. In order that such cal- portant case of large thermal conductivity and small cross sectional
culations to be made the rst return maps from Fig. 12 were ap- area of the inert core. This situation is encountered, for exam-
proximated using tenth order interpolating polynomial. The Lya- ple, in the case of carbon nanotubes used as a thermal conduct-
punov exponent dened in the ordinary way, ing element of the composite. Despite the model applied contains
a phenomenological parameter, namely the coecient describing
1
N
L = lim ln f (u f i ), (23) the linear heat exchange between the core and the shell, the nu-
N N merical facilities provided are signicant. The study of the reactive
i=1
shell-inert core conguration with one-dimensionality relaxed is in
where f(z) is the interpolating polynomial, was calculated for nite
progress.
N. It was veried that for N above 104 the inuence of the total
It is demonstrated that characteristics of ame propagation
number of iterations on L becomes negligible. Figure 13 shows
such as speed and the type of dynamical regime can be effec-
the variations of L with . One can see that the choice of the
tively controlled and manipulated, for xed chemical properties,
reference temperature affects perceptibly the level of randomness
by varying the experimental parameters of the material i.e. the
of the stochastic dynamics.
thickness of the fuel annulus deposited and the diameter of the
9. Conclusions heat conducting core. The different types of dynamical regimes in-
clude traveling, pulsating and chaotic waves. It is shown that the
The model describing the propagation of combustion waves in variation of the control parameter allow to modify the velocity of
composite energetic material having a structure of the reactive combustion wave propagation from the value corresponding to the
176 V.N. Kurdyumov et al. / Combustion and Flame 182 (2017) 167178
6
6
=3.0 =3.42
uf(n+1) uf(n+1)
5 5
4 4
3 3
2 2
2 3 4 5
ufn 6 2 3 4 5
ufn 6
6 =3.5 6 =3.7
uf (n+1) uf (n+1)
5 5
4 4
3 3
2 2
2 3 4 5
uf n 6 2 3 4 5
uf n 6
6 =4
uf(n+1)
2
2 3 4 5
ufn 6
adiabatic combustion wave in pure solid fuel to the values which bustion wave synthesis of solid materials and realization of the
are more then 5 times faster. Besides that the maximum temper- concept of chemical furnace.
ature in the energetic annulus can be adjusted from the adiabatic Complex dynamics of ame propagation are investigated. It is
ame temperature of pure solid fuel to the value exceeding it over demonstrated that the chaotic regime of combustion can be real-
30 % and more. This can be very important and benecial for com- ized. The level of stochasticity of the process measured by the Lya-
V.N. Kurdyumov et al. / Combustion and Flame 182 (2017) 167178 177
7 =3.0 to predict and which may cause thermal runaways and local over-
heating. This motivates the study of complex dynamical regimes in
uf(n+1) such materials. In the nearest future we plan to undertake an ex-
perimental investigation of combustion dynamics of the shell-core
6 energetic system made of thin metal wires and solid fuel. In such
*=0.8 conguration the ame oscillations may be detected and analyzed
with high-speed imaging and oscillations of luminosity.
*=0.5
5 Acknowledgments
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