Radiation Extinction Limit of Counterflow Premixed Lean

Methane-Air Flames
HONGSHENG GUO,* YIGUANG JU, KAORU MARUTA, and TAKASHI NIIOKA
Institute of Fluid Science, Tohoku University, 2-1-1 Katahira, A oba-ku, Sendai 980-77, Japan

and

FENGSHAN LIU
Centre for Advanced Gas Combustion Technology, Dept. of Chemical Engineering, Queen's University at Kingston,
Ontario, K7L 3N6 Canada

The application of the laminar flamelet concept to turbulent flame modeling requires a detailed understanding
of stretched laminar flames. In this study, we used numerical methods, including arc-length continuation, to
simulate the extinction characteristics of counterflow premixed fuel-lean, methane-air flames. Attention was
primarily paid to the effect of radiative heat loss on the extinction characteristics of these flames. The results
show that at medium to low values of the stretch rate, the radiative heat loss has a particularly strong impact
on the counterflow premixed fuel-lean, methane-air flames. It was also found that, in addition to the stretch
extinction limit at a high stretch rate, there exits a radiation extinction limit at a low stretch rate.
Furthermore, the relationship between these two extinction limits and the equivalence ratio is obtained. ©
1997 by The Combustion Institute

INTRODUCTION should be taken into account in the study of

Understanding the structure and extinction
characteristics of stretched laminar flames,
such as the counterflow flames, is critical to
the development and application of the lami-
nar flamelet concept to turbulent flame simu-
lation. Many researchers have studied the de-
tailed structure and the extinction characteris-
tics of these flames. Some of them have pre-
dicted and measured the stretch extinction limit
of these flames with success. However, rela-
tively few people have paid adequate attention
to the effect of radiative heat loss on the
structure and extinction characteristics of these
flames, especially for the sufficiently low stretch
rate counterflow premixed flames.
In high-temperature combustion, radiation
from flames is the predominant mode of en-
ergy transport. For instance, in boiler furnaces,
where combustion takes place, a large propor-
tion of the total heat flux from the flame to the
surrounding walls is contributed by radiation.
As a consequence, the influence of radiation
on the structure and extinction characteristics
* Corresponding author.
COMBUSTION AND FLAME 109:639-646 (1997)
© 1997 by The Combustion Institute
Published by Elsevier Science Inc.
these flames.
To date, only a few people have paid atten-
tion to the effect of radiative heat loss on the
structure and extinction characteristics of
counterflow flames. Chao and Law [1] and T'ien
[2] studied the extinction of flames caused by
the thermal radiation from a condensed sur-
face by asymptotic theory. They found that the
flame will extinguish at a low stretch rate when
the radiative heat loss from the condensed fuel
surface exists. However, both these papers ig-
nored the gas-phase radiation. Liu and Rogg
[3] numerically studied the influence of radia-
tion heat loss on the counterflow diffusion
flame, and showed that at a low stretch rate
radiation has a strong impact on the flame
structure. In the study of NO x emission of
diffusion flames, Hewson and Williams [4]
found that both the flame temperature and
NO x emission index fall as the stretch rate
decreases from a critical value, when the radia-
tive heat loss is considered. In the study on the
effects of radiation heat loss on the structure
of stretched diffusion flamelets, Liu et al. [5]
found that there exists a new extinction limit
of small dissipation rate when the radiative
heat loss from the flame is taken into account.
Egolfopoulos [6] studied the radiation effects
0010-2180/97/$17.00
PII S0010-2180(97)00050-3
640
on steady and unsteady stretched laminar
flames, and indicated that radiation is impor-
tant for near-limit premixed flames and for
weakly-stretched diffusion flames. However,
the study was not extended to sufficiently low
stretch rates.
Platt and T'ien [7] first investigated the ex-
tinction of counterflow premixed flames at low
stretch rates, and found that the flame extin-
guishes at a low stretch rate. However, a sim-
ple one-step overall reaction mechanism, which
cannot consider the effects of the chain-
branching and the chain-terminating process,
and constant transport properties were used in
the paper. The experimental study carried out
by Maruta et al. [8], under microgravity condi-
tions, indicated that, in addition to the stretch
extinction, which occurred at a high stretch
rate, the flame extinction also happened when
the stretch rate decreased to a sufficiently low
value. Therefore, it is necessary to employ a
detailed chemistry and complex transport
properties to further study whether, in addition
to the stretch extinction limit at a high stretch
rate, there exists another extinction limit at a
low stretch rate for counterflow premixed
flames, which may be caused by the radiation
heat loss from the flame, and to discover what
is the mechanism of this extinction.
In the present study, numerical studies of
counterflow premixed fuel-lean, methane-air
flames were conducted to gain insight into the
extinction characteristics of counterflow pre-
mixed fuel-lean, methane-air flames, with spe-
cial attention paid to the effect of the radiative
heat loss from flames. A series of calculations
were performed for different values of the
equivalence ratio. The arc-length continuation
method was used to obtain the extinction limit.
The emphasis is on the low stretch rate at low
equivalence ratio region.
The present numerical computations of
counterflow premixed flames were conducted
with complex transport properties and detailed
chemical kinetics. The necessary thermochemi-
cal and transport properties were obtained
from CHEMKIN data base [9]. The adopted
numerical scheme was basically developed by
Smooke et al. [10] for the simulation of one-di-
mensional premixed flames.
The most important attention in our calcula-
H. G U O ET AL.
tion is paid to ascertain whether, in addition to
the stretch extinction limit, the radiation heat
loss can lead to another extinction limit at a
low stretch rate, i.e., whether a radiation ex-
tinction limit at a low stretch rate exists in
counterflow premixed flames. We expect that
this radiation extinction limit may strongly de-
pend on the value of the equivalence ratio.
Another purpose of this study is to understand
the mechanism of the extinction observed ex-
perimentally [8].
NUMERICAL MODEL
Governing Equations and Solution Procedure
The flame we modeled can be produced by two
counterflowing reactant streams which emerge
from two coaxial jets. In the neighborhood of
the stagnation point produced by these flows, a
chemically-reacting boundary layer is estab-
lished, as shown in Fig. 1.
The present simulation for counterflow pre-
mixed flames assumes a laminar stagnation
point flow. The boundary layer approximation
was used in this calculation. The governing
equations for mass, momentum, chemical
species and energy can be found elsewhere
[11]. Cylindrical coordinates were used in our
simulation. The only difference between this
work and that conducted by Giovangigli and
Smooke [11] is the energy conservation equa-
tion, in which we retained the sink term due to
~y
Fig. 1. Counterflowpremixed flame configuration.
RADIATION EXTINCTION LIMIT
the thermal radiation. In the present study, all
these conservation equations were transformed
into a set of ordinary differential equations.
For the sake of brevity, we give only the energy
conservation equation here:
dT dT
p c i , ~ t + pVCp dy
=--
dy A Ty - ~'~hkwkM k
KK dT
- ~ PYkCpkVk--SS, +
uy
qr (1)
k=l
where qr is the sink term due to the thermal
radiation which will be described in the next
subsection, and KK is the number of species.
Because the C 1 path is the principal channel
for fuel-lean, methane-air flames, especially
for the flame speed and the extinction, the C 1
elementary reaction mechanism, which in-
volves 58 reactions and 18 species, was em-
ployed in this calculation. It is given by Kee
et al. [12] and can accurately reproduce the
experimental data over extensive concentration
and pressure ranges tested in [13].
Our calculation was carried out basically by
using the CHEMKIN code developed by
Smooke et al. [10, 12, 14]. Windward differ-
ences were used for the convective term.
Adaptive refinement of meshes was done. The
arc-length continuation method [11, 15] was
used to obtain the extinction limits.
The Sink Term of the Energy Equation
In the present investigation, attention was paid
to the influence of radiative heat loss on the
extinction limit of counterflow premixed fuel-
lean, methane-air flames.
Based on the optically thin approximation,
the sink term due to the radiation, qr, may be
calculated as [16]:
qr = - 4 o ' k p ( T 4 - T 4) (2)
where o- is the Stefan-Boltzmann constant; kp
is the Planck mean absorption coefficient; To
is the ambient temperature, and T is the in-
stantaneous local temperature.
The Planck mean absorption coefficient ac-
counts for the absorption and emission from
641
the gaseous species CO2, H20 , CO and CH 4,
and is expressed as:
kp = p~.~xikp, i (3)
where p is the pressure (atm), and kp, i and xi
denote the mean absorption coefficient and
mole fraction, respectively, of absorbing and
emitting species. The quantity, kp,i, c a n be
given as in [17].
Experimental study [8] showed that even at a
low stretch rate, twin flames extinguish by
merging with each other. The maximum dis-
tance between twin flames at the low equiva-
lence ratio is very small (less than 20 mm).
Therefore, the optically thin assumption for
the radiation is basically appropriate near the
extinction limit.
RESULTS AND DISCUSSION
We performed a series of calculations of
the flame extinction limits of counterflow pre-
mixed fuel-lean, methane-air mixtures at at-
mosphere-pressure with the equivalence ratio
varying between 1.0 to 0.421. Unless it is ex-
plicitly indicated, all calculations were con-
ducted with the radiative heat loss included.
Figure 2 shows the fame temperature versus
the stretch rate, a (l/s), for various equiva-
lence ratios. We can see from this figure that
for each equivalence ratio, as the stretch rate
increases from a value at which the flame
temperature is the highest, the flame tempera-
ture decreases until the extinction limit is
reached at the point of the vertical tangency.
We name this extinction limit at a high :stretch
1500
ff ~400
1300
1200 J f I J l : I
2O 40 60 80 100
Stretch rate, 1/s
Fig. 2. Flame temperature as a function of the stretch rate
for various equivalence ratios.
642
rate the "stretch extinction limit." Many re-
searchers have studied this stretch extinction
limit theoretically a n d / o r experimentally [11,
15]. Therefore, there is no need of detailed
explanation for this limit here again.
A new phenomenon shown in Fig. 2 is that,
as the stretch rate decreases from the maxi-
mum flame temperature point, the flame tem-
perature for each equivalence ratio also de-
creases and, finally, another extinction point,
where d T / d a ~ oo, is reached on the left por-
tion of the curves. A detail of Fig. 2 at low
stretch rates is given in Fig. 3, which shows the
point of the vertical tangency at a low stretch
rate more clearly. These results indicate that,
in addition to the stretch extinction limit men-
tioned above, there is another extinction limit
at the low stretch rate. We name this extinc-
tion limit at the low stretch rate the "radiation
extinction limit." A detailed discussion of this
radiation extinction limit at the low stretch
rate will be given in the following section.
Radiation Extinction Limit
Figures 2 and 3 clearly show that there is
another extinction limit at the low stretch rate,
in addition to the stretch extinction limit at the
high stretch rate. It can be seen that the tem-
perature at the radiation extinction limit is
lower than that at the stretch extinction limit.
Figure 4 shows the comparison between the
case in which the radiative heat loss is consid-
ered and the case in which the radiative heat
1 3 . . . . . . .
~ 1260
lz2o
1200 i , I I * ,
1 2 ' S ' 10
Stretchrate, 1Is
Fig. 3. Amplified graph in the vicinity of the radiation
extinction limits.
H. G U O ET AL.
1400 l l ' ' ' ' i i
~ 1300
1200
~D @=0.43
--O-- R a d i a t i o n h e a t loss Ignored
---e-- Radiation heat loss included
1100 I i I • , , ,l I
s 10 2o
Stretch rate, l/s
Fig. 4. Comparison between the case in which radiative
heat loss was considered and the case in which radiative
heat loss was ignored.
loss is ignored for the equivalence ratio of 0.43.
It can be seen that when we did not consider
the radiative heat loss, as the stretch rate in-
creases the flame temperature first slightly rises
to a maximum point, then falls toward the
stretch extinction limit. The flame temperature
difference between these two cases increases
with the decrease of the stretch rate. The slight
decrease of flame temperature at the low
stretch rate for the case in which radiative heat
loss was ignored is due to the influence of the
Lewis number, which has been discussed by
many researchers both experimentally and the-
oretically [18-20].
However, if the radiative heat loss from the
flame is not taken into account, we can easily
imagine that the flame would not extinguish at
a low stretch rate, as shown in Fig. 4. Conse-
quently, we can say that the extinction at the
low stretch rate for counterflow premixed fuel-
lean, methane-air flames is caused by the ra-
diative heat loss. This is why we call this ex-
tinction limit at the low stretch rate "radiation
extinction limit," being different from the
"stretch extinction limit" at the high stretch
rate in the physical mechanism.
The radiation extinction mechanism at the
J low stretch rate is as follows. First, as the
stretch rate decreases from the maximum flame
temperature point, the flame zone first rela-
, , tively thickens, and thus the heat release rate
per unit volume of the flame zone decreases.
From Eq. 2, the radiative heat loss is propor-
tional to volume fractions of absorbing and
RADIATION EXTINCTION LIMIT
emitting gases, which are not significantly af-
fected by the stretch rate. Hence, the rate of
radiative heat loss per unit volume is not
strongly dependent on the stretch rate. As a
result, the ratio of the sink term due to the
radiative heat loss, to the heat release term in
the Eq. 1, increases, and the temperature of
the flame falls as the stretch rate decreases. To
demonstrate this, we define a parameter, rr,
which may be called the radiation fraction, as:
r/= f Lqr dy ~. hlctol~Mkdy (4)
k=l
where h k represents the specific enthalpy of
the kth species; tok, the molar rate of produc-
tion of the kth species per unit volume; L, the
distance from the stagnation plane to the
burner exit, and M k, the molecular weight of
the kth species. Figure 5 plots rf versus the
stretch rate for the equivalence ratio of 0.48. It
should be noted that the fraction of radiation
increases rapidly as the stretch rate decreases.
However, rf equals to only 23.4% at the stretch
rate of 1.1 l / s , which is near the radiation
extinction limit. Such a small value of rf can-
not lead to the flame extinction, so there must
be another physical factor resulting in the radi-
ation extinction.
Second, the flame zone moves forward to the
burner as the stretch rate decreases at the
beginning, and so the downstream zone be-
tween twin flames with a higher temperature
and higher concentration of COe and H 2 0
becomes thicker. As a result, radiative heat
loss from this zone increases, which then leads
u I u I
,~
20
..~
cI,=0.48
~ o , J , I - ' ~ ~ , a O
o 20 40 60
Stretch r a t e , 1/s
Fig. 5. F r a c t i o n of r a d i a t i o n as a function of the stretch
r a t e for the e q u i v a l e n c e r a t i o of 0.48.
643
to the fall of temperature between twin flames.
Consequently, conductive heat loss from the
flame toward the stagnation plane increases,
which further lowers the temperature of the
flame. There would not be this term of conduc-
tive heat loss if we did not consider the effect
of the radiative heat loss. This is another phys-
ical factor leading the radiation extinction.
Both of these two factors accelerate the
drop of the flame temperature more quickly as
the stretch rate decreases from the maximum
flame temperature point.
At a sufficiently low stretch rate, the sum of
the radiative and conductive heat loss is so
strong that the flame temperature becomes
very low. Therefore, the flame propagation
speed, with a decrease rate which, because of
the drop of the flame temperature, is higher
than the decrease of the reactant flow rate,
becomes slower than the reactant flow rate.
Consequently, the reaction zone moves back to
the stagnation plane again, and the reaction
cannot be completed, leading to the radiation
extinction. The distance between twin flames,
based on the maximum temperatures in twin
flames versus the stretch rate for the equiva-
lence ratio of 0.48 is shown in Fig. 6. It should
be noted that a decrease of the stretch rate
leads to the distance between flames decreas-
ing rather than increasing near the radiation
extinction limit. This radiation extinction pro-
cess is consistent with the experimental obser-
vation [8].
To demonstrate the radiation extinction pro-
cess, the mole fractions of CO and OH, and
r . . . .
•1 • r . . . . I
~2
~4
(P=0.48
=2
Flammable region
,1 i I I
s 10 so 100
Stretch r a t e , l / s
Fig. 6. T h e d i s t a n c e b e t w e e n twin f l a m e s versus the stretch
r a t e for ~b = 0.48.
644 H. G U O ET AL.

the flame temperature along the axial distance
for three typical values of the stretch rate
where the equivalence ratio equals 0.48, are
plotted in Fig. 7. The flame zone is close to the
stagnation plane at the stretch rate of 40.0 1/s.
Then, the reaction zone moves towards the
burner exit at the stretch rate of 6.0 1/s. When
the stretch rate is further reduced to 1.1 1 / s
(which is near the radiation extinction limit for
this equivalence ratio), the reaction zone moves
again to the stagnation plane, but with incom-
plete combustion.
Flammable Region of Counterflow
Premixed Flame
From Figs. 2 and 3, we note that both the
stretch extinction limit and the radiative ex-
tinction limit change for different values of the
equivalence ratio. We plotted all the stretch
extinction limits and the radiation extinction
i "1 i i
kd l.fd)0 (A)
limits in the a-th plane; a C-shaped extinction
limit curve was dearly formed, as shown in Fig.
8. In this graph, the flammable region is
bounded by two branches of extinction limit
boundaries: the stretch extinction limit branch
and the radiative extinction limit branch. For
the equivalence ratio between approximately
0.421-0.48, if we start with a flame, the stretch
extinction limit can be reached when the
stretch rate is increased and the radiation ex-
tinction limit can be reached when the stretch
rate is decreased. At approximately ~b = 0.421,
the two branches merge at one point, which we
call "flammability limit of counterflow fuel-lean
premixed flames." For the equivalence ratio
below the value specified by this point, a steady
stagnation-point premixed flame cannot be es-
tablished regardless of the values of the stretch
rate. This low lean limit for the counterflow
premixed methane-air flames is lower than
that for the plane premixed flames without
stretch effect, which is approximately 0.49, ob-
tained by Law and Egolfopoulos [21].
The radiative extinction limits for the equiv-
| I ' i i w I ' ' ' ' -I
alence ratio greater than 0.48 may exist at a
a:40.0 l/s
.......... a=6.0 1/s :""'"['~
J very low stretch rate, or do not exist. Because
the calculation at very low stretch rates is quite
difficult, we have not obtained the radiation

J-I00 0.02 ' ' ' ' I ' ' ' ' I . . .
/'/1
.
extinction limits for the value of the equiva-
lence ratio higher than 0.48.
The comparison of the present numerical
results with the experimental results [8, 22] is
(13) shown in Fig. 9, in which the velocity gradient
0.015 a=40.0 l/s in experiments (U/L, where U is the velocity
,~ ............ *=6.0 its
.~ 0,01 ....... a=l.l 1/s

8 0.005 (I)=0.48 /~ lO3

Methane/air premixed flame
, , , , I , , , _L..---I''"~'.J', ,

8xlO ~ i i i i i i i i , i i m i ' 4 10~

000•
= (C)

1
6xlO-4 - - a=40.O lls Stretch extinction limit
............ a=6.0 l/s 101
0•
4×10-4 ....... a=l.1 1/s ,~ • Radiation extinction limit

o
2×10.4 @--0.48
!! \
~ 10o i .../.,
[ Flammability limit of
i/ eounterflow premixed flame
-3 -1 -2o 10-t I , t I I , i i I
y, c m 0.4 0.5 0.6
Fig. 7. Temperature, C O and O H mole fractions as a Equivalence ratio
function of axial distance for three typical values of stretch Fig. 8. C-shaped curve for counterflow premixed fuel-lean,
rate at ~b = 0.48. (a) Temperature; (b) CO; (c) O H . m e t h a n e - a i r flames.
RADIATION EXTINCTION LIMIT
.~ 10 4
' I ' I ' The present result is qualitatively consistent
•~ 10~
g~
Oo
10 2
umerlcal results
.. 10l
iA OElaruta et al., [81)
O Experiments in normal gravity
~ 10a (Law et al., [20])
'~ Present supplementary
experiments In normal gravity
~ 1 0 -l I , I , t J 1 , I
0.4 0.6 0.8
E q u i v a l e n c e ratio
Fig. 9. Comparison of extinction limits with experimental
results.
at the nozzle exit and L is the distance be-
tween the nozzle exit and the stagnation plane)
corresponds to the value 2a (a is the stretch
rate). Supplementary experiments in normal
gravity in this graph were carried out to con-
firm some extinction data at the equivalence
ratio around 0.50 to 0.55. The burner system
and the mixture supply system are the same as
those used in [8] and [23], respectively. This
C-shaped extinction limit curve is qualitatively
consistent with the experimental observation.
CONCLUSION
The effects of radiative heat loss on the coun-
terflow premixed fuel-lean, methane-air flames
have been numerically investigated with C 1
chemistry and complex transport properties.
The results show that the radiative heat loss
has a strong impact on the flame structure at
low values of stretch rate. It is found that the
radiative heat loss will lead to the flame extinc-
tion at a low stretch rate. For counterflow
premixed methane-air flames, the lean flam-
mable region is bounded by a C-shaped curve.
The upper part of the curve is the stretch
extinction limit and the lower part of the curve
is the radiation extinction limit. These two
extinction branches merge at one point, which
indicates the lean flammability limit of coun-
terflow premixed methane-air flames. For the
equivalence ratio below the value specified by
this point, a steady stagnation point premixed
fuel-lean, methane-air flame cannot be estab-
lished.
645
with the experimental result.
The authors thank Mr. Atsutaka Honda for
carrying out the supplementary experiments in
normal gravity.
This work was performed under the manage-
ment of the Japan Space Utilization Promotion
Center as part of the R & D project of Advanced
Furnaces and Boilers supported by the NEDO
(New Energy and Industrial Technology Develop-
ment Organization).
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