International Journal of Hydrogen Energy 29 (2004) 1365 – 1370

www.elsevier.com/locate/ijhydene

Optimization of hydrogen production by +ltration combustion

of methane by oxygen enrichment and depletion
J.P. Bingue, A.V. Saveliev, Lawrence A. Kennedy∗
Department of Mechanical and Industrial Engineering, University of Illinois at Chicago, Chicago, IL 60607, USA

Received 7 July 2003; received in revised form 15 December 2003; accepted 2 January 2004

Abstract
Transient +ltration combustion waves formed in a porous matrix of randomly arranged alumina pellets are studied experi-
mentally for rich and ultra-rich methane/air waves with oxygen enrichment and depletion. A single +ltration velocity (12 cm=s)
was used and the mixture equivalence ratio was varied from 1 to 3.5. The air and oxidizer content were adjusted to retain the
+ltration velocity constant for each equivalence ratio. Six oxidizer compositions (10%, 15%, 21%, 25%, 30%, and 35% O2 )
were comparatively analyzed focusing on combustion temperatures, combustion wave velocities, major and minor products of
combustion. The studied range of equivalence ratios covered the underadiabatic (upstream) and superadiabatic (downstream)
regimes of transient +ltration waves where combustion temperatures are less than and greater than adiabatic temperatures,
respectively.
? 2003 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights reserved.

Keywords: Hydrogen production; Filtration combustion; Porous media

1. Introduction hydrogen production. While eFcient and popular, SMR re-

Recent insights into pollution control have dubbed hydro-
gen as the fuel of the future. It is set to provide the energy to
propel our everyday mobility, power our homes and indus-
try; therefore hydrogen will not only be the engine behind
our economy, it will be the economy. At present, hydrogen
is used as a major intermediate in many chemical applica-
tions such as the processing of heavy feedstock, or the man-
ufacturing of ammonia-based fertilizers and methanol. For
the moment, the available processes of producing hydro-
gen from certain hydrogen containing species are both la-
borious and capital intensive. Historically, steam reforming
(SMR) of some light hydrocarbons, mostly methane, and
catalytic partial oxidation (CPOX) of light and heavier fuels
has been the most popular methods of hydrogen extraction.
Of these two processes, SMR accounts for more than 80% of
∗ Corresponding author. Tel.: +1-312-996-2400; fax: +1-312-
996-8664.
E-mail address: lkennedy@uic.edu (L.A. Kennedy).
quires rather large plants for economic viability, hence sub-
stantial capital cost. The latter method does not require the
substantial investment in capital but the technical practical-
ities are yet to be overcome. CPOX requires high tempera-
tures that shortens catalyst life. Firstly, catalytic operations
requires downtime that disrupts operations. For the projected
utilization of hydrogen, simpler and eFcient processes will
have to be found. One such solution is superadiabatic de-
composition of light hydrocarbons in a porous media.
The theory of +ltration combustion involves a new type
of Game with exothermic chemical transformation during
Guid motion in a porous media. Its base rose out of the the-
ory of excess enthalpy Game promulgated by Egerton et al.
[1] and Weinberg [2] almost 40 years ago in a theoretical
demonstration that combustion temperatures in a system can
be higher than the adiabatic temperature if an energy feed-
back system is available for the incoming reactants [3]. As
an internally self-organized process of heat recuperation, +l-
tration combustion of gaseous mixtures in porous media dif-
fers signi+cantly from homogeneous Games. This diJerence
is attributed to the following two main factors: the highly

0360-3199/$ 30.00 ? 2003 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights reserved.
doi:10.1016/j.ijhydene.2004.01.002
1366 J.P. Bingue et al. / International Journal of Hydrogen Energy 29 (2004) 1365 – 1370

developed inner surface of the porous medium results in ef- hydrogen. Thorough reviews of +ltration combustion have
+cient heat transfer between gas and solid, and dispersion been produced by Howell et al. [20] and most recently by
of reactants and products in the porous media increases ef- Kennedy et al. [21].
fective diJusion and heat transfer in the gas phase. This The present work is a comprehensive study of tran-
process is responsible in ensuring stable combustion waves sient +ltration combustion in an inert porous media. The
over a wide range of reactant velocities, air–fuel ratios, and emission characteristics of rich and ultra-rich combus-
power loads. Within the context of porous combustion, two tion waves formed under +ltration of oxygen enriched
ideas have been presented: stationary and transient combus- and depleted air/methane mixtures in an inert packed bed
tion zone systems. The +rst approach is widely exploited are studied experimentally. With the extension and con-
in radiant burners and surface combustor–heaters where the traction of the combustion zone by oxygen enrichment
combustion zone is stabilized within the +nite element of and depletion [22], the products of the partial oxida-
the porous matrix. This area includes porous radiant burn- tion combustion regime can be modi+ed advantageously;
ers for Joule heating advanced by Tong and Sathe [4] and speci+cally, the water–gas shift reaction to reduce the
Rumminger et al. [5], porous burners with ultra-low pollu- amount of water in the product not only is favorable
tant emission characteristics by Trimis and Durst [6]. The to hydrogen (H2 ) yield but also reduction of carbon
surface combustor–heater system was developed by Khinkis monoxide (CO) concentrations. Furthermore, generalized
et al. [7] and Mohamad et al. [8]. models can be validated.
The second (transient) approach involves a traveling wave
where the unsteady combustion zone freely propagates as a
wave either in the downstream or upstream direction within 2. Experimental approach
the packed bed. Strong interfacial heat transfer results in
The experimental apparatus consists of three major sec-
a low degree of thermal non-equilibrium between the gas
tions: Gow control system, the reactor itself, and data ac-
and solid; the relative displacement of the combustion zone
quisition components (Fig. 1). The reactor or combustion
generates positive or negative enthalpy Guxes between the
chamber is made up of a 43 cm long quartz tube with
reacting gas and solid phase. As a result, observed com-
bustion temperatures can be signi+cantly diJerent from the
adiabatic predictions and are controlled mainly by the re-
action chemistry and heat transfer mechanism. These con-
ditions correspond to the low-velocity regime of +ltration
gas combustion, according to classi+cation given by Babkin
[9]. The upstream wave propagation, countercurrent to reac-
tant Gow, results in underadiabatic combustion temperatures
[10], while the downstream propagation of the wave leads to
the combustion in superadiabatic regime with temperatures
much in excess of the adiabatic one [11].
Lately, a number of researchers have undertaken the
challenges of understanding the fundamentals of transient
+ltration waves. Korzhavin et al. [12] studied the regime
transition from slow to high velocity due to various dy-
namic parameters (e.g. pressure, vessel size) of the porous
media system and noted that turbulence accelerates the
combustion process as observed by a rise in the pressure
gradient at the Game front. Minaev et al. [13] studied the
instabilities of a propagating front in the concurrent direc-
tion of gas Gow such that the wave is inclined in relation to
the perpendicular Gow but stated that wave inclination does
not exist in counterGow propagation.
The idea of using rich +ltration combustion waves for the
purpose of fuel reformation has gained new insight from
the works of Drayton et al. [14] and Kennedy et al. [15,16].
Various other researchers [17,18] have used a feedback
recuperative system to attain a self-sustainable combustion
wave in the range of equivalence ratios () from 2 to 3
for methane/air Game. Saveliev et al. [19] performed ex-
periments with hydrogen/air mixtures and reported stable
combustion waves for mixtures containing as low as 3% of Fig. 1. Schematic of the experimental setup.
 J.P. Bingue et al. / International Journal of Hydrogen Energy 29 (2004) 1365 – 1370 1367

inner and outer diameters of 38 and 42 mm, respectively. 1700

The small internal diameter of the reactor is purposely se- 2.50
2.
lected to suppress development of inclination instabilities,
2.00
2.0
experimentally observed for downstream propagating waves

Combustion Temperature, K
1650
[14]. The tube’s interior is lined with a 3 mm thick layer
1.75
1.
of high-temperature ceramic +ber insulation to protect the
quartz from the constant thermal expansion of the solid me- 1600
dia under +ring conditions. The outer portion of the tube is
insulated by an 8 cm thick layer of the same insulation start-
ing from the reactor’s exit and 40 cm downward covering 1550
the diagnostic section and thus creating a one-dimensional 1.25
1.
structure of the combustion waves by ensuring negligible ra-
dial temperature gradients across the combustion zone. The 1500
reactant metering system consists of a set of MKS mass Gow
controllers (Model 1179A, MKS Inc.) for accurate measure-
φ=1.00
1.00
ment of the various reactants (98% pure methane, oxygen, 1450
nitrogen, and dry laboratory air). 5 10 15 20 25 30 35 40
Mixtures of methane/air and nitrogen or oxygen enriched Oxygen Content of Oxidizer , %
air were introduced from the mixing chamber at the reac-
tor’s bottom via a water-cooled metal plug at the reactor’s Fig. 2. Combustion temperature as function of oxygen content of
base and ignited at the reactor’s mouth. The range of tested oxidizer for equivalence ratios 1.0, 1.25, 1.75, 2.0, and 2.5.
equivalence ratios, , was swept at each oxygen index and
single +ltration velocity (12 cm=s). For each tested equiva-
lence ratio, the total mixture Gow rate and +ltration velocity 0.006
were kept constant adjusting both the fuel and the oxidizer 10%
Gow rate. Errors for measured temperatures and calculated 0.004 Air
velocities were less than 5%. Combustion temperature data
Combustion Velocity, cm/s

were collected by a set of six S-type thermocouples shielded

0.002
inside a multi-bore ceramic tube running axially in the cen- 15
ter of the quartz tube. The gas was sampled through an in-
ert ceramic probe dipped by 3 cm into the packed bed and 0
connected to a gas chromatograph.
-0.002

3. Results and discussion

3.1. Combustion temperature and propagation rate
The actual measured temperature is the porous matrix
temperature. Fig. 2 shows the temperatures as a function of
the oxygen content of the oxidizer (OCO) for equivalence
ratios 1, 1.25, 1.75, and 2.50. The lower equivalence ratios
(1 and 1.25) display behaviors counter to homogeneous
Games; here temperatures of under-oxidized mixtures are
considerably higher than temperatures for air and mixtures
where the oxidizer contains 35% oxygen. For OCO 10%,
the combustion temperature at equivalence ratio of 1.25 is
1636 K as compared to 1552 K for air and 1549 K for
30%. For the same equivalence ratio, the temperature rose
to 1571 K by 35% due to combustion zone displacement
eJect (Fig. 3). For  = 1:0, the temperature drops contin-
uously from OCO 15% to 30%. Above equivalence ratio
1.50, the combustion temperature is almost independent of
the mixture’s oxygen content since there exists no oxygen
beyond the initial combustion zone.
The relative energy Gux inside the combustion zone,
and hence mixture composition, eventually decides the
-0.004 35
-0.006 30
25
-0.008
1 1.5 2 2.5 3
Equivalence Ratio
Fig. 3. Combustion wave velocity with respect to equivalence ration
for six oxidizer indices.
propagation rate and direction of the combustion. Due to
gas and solid interaction, the Game velocity inside a media
can be 10 times greater than homogeneous premixed Game.
The rate and direction of propagation of the combustion
zone is of great importance in this type of system since the
residence time will have great inGuence on the composition
of the combustion products. Fig. 3 displays the combus-
tion velocity as a function of equivalence ratio for all the
tested OCOs with air as the reference oxidizer (OCO =
21%). Positive velocities relate concurrent movement of the
1368 J.P. Bingue et al. / International Journal of Hydrogen Energy 29 (2004) 1365 – 1370
25
35
20
30
Hydrogen, %
Air
15
10
25
15
5
10%
0 0
1 1.5 2 2.5 3 3.5
Equivalence Ratio
Fig. 4. Concentration of hydrogen in the product stream for all
tested oxygen indices.
combustion zone and the gas whereas the negative ones are
the countercurrent displacement. Since each OCOs have
diJerent energy content at a particular equivalence ratio, the
propagation rate of the combustion zone will be diJerent.
Therefore, the equivalence ratio point of transition between
positive and negative displacement of the combustion zone
will also occur at diJerent point for a particular OCO. The
reference OCO air has a transition point at approximately
 = 1:65, coincidentally its upper Gammability limit for a
homogeneous methane/air Game. Lacking suFcient energy,
the lowest tested OCO, 10, never propagates countercurrent
to the reactant Gow direction. OCO of 15% has a transition
point approximately at equivalence ratio 1.25. As one goes
to higher OCOs, hence more energetic mixtures, the tran-
sition points are shifted to higher equivalence ratios. If all
the equivalence ratios for OCO 35% were tested, one can
safely assume that its counter Gow motion would have been
the fastest recorded and the highest transition equivalence
ratio.
3.2. Combustion products
The products of combustion were expected to be diJerent
for rich and ultra-rich mixtures; hence products were sam-
pled in both regimes. Of utmost importance in this work is
the amount of hydrogen in the products of combustion and
the ability of this type of combustion system to convert a rel-
atively greater portion of the methane into hydrogen rather
than water or higher C2 -based hydrocarbons. Fig. 4 shows
that the product stream can contain as much as 25% hydro-
gen for OCO 35% at  = 2:75. In this ultra-rich regime,
the products of combustion are controlled by the equilib-
rium temperature and residence time. At  ¿ 2:5, this pro-
cess can be characterized as fuel reformation rather that
20
35
15
Carbon Monoxide, %
30
25
Air
10
15
5 10%
4 1 1.5 2 2.5 3 3.5 4
Equivalence Ratio
Fig. 5. Levels of carbon monoxide in product with respect to
equivalence ratio.
combustion such that a stable thermal process exists with
a minute concentration of oxygen. This type of system is
possible by the unconstrained movement of the combustion
zone to recuperate its energy from the porous matrix.
For all the OCOs, hydrogen as a product is minimum in
the normal combustion regime and maximizes in the par-
tial oxidation regime, 2 ¡  ¡ 3, with higher equivalence
ratios favoring higher OCOs. Beyond this region the hydro-
gen yield drops signi+cantly especially for OCO 25%. In
these equivalence ratio ranges, the production of hydrogen
is helped by the water–gas shift reaction. The addition of
small amounts of oxygen can shift this water–gas reaction
window into higher of equivalence ratios. Therefore, the ad-
dition of oxygen in the oxidizer stream oJers the possibility
of reducing the concentration of water as a product. The dis-
advantage of such a system is the production of soot. Further
analysis of the results shows that CO (Fig. 5) is maximized
much earlier. A closer look would reveal that the maximum
amount of CO is slightly shifted backward as compared to
the maximum for hydrogen for any particular OCO. The
relatively high CO output on or near stoichiometry ( = 1)
is due to the lower combustion temperature (Fig. 2) which
does not permit the total oxidation of CO to CO2 .
Signi+cant amount of methane in the product stream be-
gan to appear past an equivalence ratio of 1.5. Fig. 6 show
that generally the lower OCOs have lower levels of leftover
methane for all rich mixtures. That trend is expected for the
lower OCOs since the temperature is generally higher in that
region. The ultra-rich mixtures, speci+cally =2:75 and 3.0,
do not follow the general trend where a value of 5% is ob-
tained for air =2:75, and twice as much for OCO=25, then
approximately 9% for 30% and 35% OCO. The trend for
=3:0 is similar. The opposite eJect was observed by Wein-
berg and Brophy [17]. In these regimes, the formation of C2
 J.P. Bingue et al. / International Journal of Hydrogen Energy 29 (2004) 1365 – 1370 1369

15 80

Carbon Monoxide Conversion, %

10%
70
3.0
Unreacted Methane, %

10 60 Air
2.75

50 15
2.25
25
30
40 35
5 1.75

φ = 1.5 30

0 20
1 1.5 2 2.5 3 3.5 4
5 10 15 20 25 30 35 40
Equivalence Ratio
Oxygen Content of Oxydizer, %
Fig. 8. Conversion of carbon molecule in the fuel to carbon
Fig. 6. Graph of unreacted methane as a function of oxygen content monoxide.
in the oxidizer.

In the range of equivalence ratios 1.5–2.0, conversion rates

45 vary from 35% to 39%. The most eFcient range with re-
spect to hydrogen conversion is between 2.0 and 2.5. Be-
40 yond equivalence ratio 2.5, the hydrogen conversion rate
drops steeply to less than 30% except for air. The conversion
Hydrogen Conversion,%

35
30
10%
25
20
15
10
5
1 1.5
Fig. 7. Conversion of available hydrogen in reactant to molecular
hydrogen.
hydrocarbons [14,15] is ascertained and those generally give
way to soot formation as observed in the present work and
observations of Itaya et al. [18]. With a relatively large quan-
tity of unreacted methane at the higher OCOs, the eFciency
of the inert porous media to convert methane into hydro-
gen lie in the low OCO ranges. Fig. 7 shows that the single
highest conversion rate (42%) is registered for 15% OCO at
 = 2:25 where the conversion rate is de+ned as the amount
of hydrogen in the products divided by twice the input
methane. As expected, the conversion rate is less than 30%
for equivalence ratios less than 1.5 at all oxygen indices.
Air trend of available carbon to carbon monoxide is more uni-
form than the trend for hydrogen conversion. Fig. 8 shows
that minimal concentration of the fuel is converted to CO
35 near stoichiometry. This factor is due to relative abundance
30
of oxygen to form water and help oxidize CO to carbon
dioxide. The optimization of CO does not occur until equiv-
15 alence ratio is 1.5. Beyond this regime, partial oxidation is
the main mechanism of combustion. The water–gas shift re-
25 action is the major factor responsible for decreased conver-
sion. In observing Figs. 6 and 8, the indication would be that
another factor is responsible for the low conversion to CO
2 2.5 3 3.5 4 past  = 2:5. In this zone, the formation of higher hydrocar-
bon is the most likely avenue for the fuel to exit the reactor
Equivalence Ratio
as noted by the low level of unreacted methane at higher
OCO. By careful analysis of the product, one can deduce that
there exists three distinct regimes of combustion in traveling
from rich to ultra-rich: combustion (1:0 ¡  ¡ 1:5), partial
oxidation (1:5 ¡  ¡ 2:5), and fuel reformation ( ¿ 2:5).
4. Conclusions
Rich and ultra-rich +ltration combustion waves formed in
a packed bed of randomly arranged alumina pellets are stud-
ied experimentally. The studied range of equivalence ratios
from 1.0 to 3.5 covers the superadiabatic and underadia-
batic combustion waves formed in the rich and ultra-rich re-
gions. With methane as fuel, six oxidizer compositions were
selected. The six-oxidizer compositions (10%, 15%, 21%,
25%, 30%, and 35%) are comparatively analyzed focusing
1370 J.P. Bingue et al. / International Journal of Hydrogen Energy 29 (2004) 1365 – 1370
on combustion temperatures, combustion wave velocities,
and main products of partial oxidation: H2 , CO.
It is found that the peak combustion temperature drops
with oxygen enrichment while the absolute Game propa-
gation rate increases. In rich mixtures, temperature diJer-
ences of almost 100 K exist for mixtures of various oxygen
contents. The reverse variation of adiabatic and combus-
tion temperatures strongly aJects regimes of superadiabatic
(downstream) and underadiabatic (upstream) wave propa-
gation. For an OCO of 10%, the Game is found to be to-
tally superadiabatic in the whole range of equivalence ratios
tested. Signi+cant extension of underadiabatic Game region
is observed for high OCOs.
Products of combustion are sampled and analyzed com-
paratively. It is observed that mixtures with higher oxy-
gen content in the oxidizer stream generate higher amounts
of hydrogen and carbon monoxide. The overall region of
higher yield is between 2 ¡  ¡ 3. Furthermore, it was in-
ferred that peak hydrogen emission is shifted toward higher
equivalence ratio for successively higher OCOs with 35%
OCO generating almost 25% H2 of the total products at
an equivalence ratio of 2.75 but OCO of 15% oJers the
highest rate of methane conversion to hydrogen. CO emis-
sions behave similar to hydrogen with maximum between
1:5 ¡  ¡ 2:5. Unreacted methane appears in the product
stream for  ¿ 1:5 where lower OCOs produces lower lev-
els of unreacted methane for all rich mixtures. The sam-
pled products help distinguish the three distinct regimes of
combustion in sequence from rich to ultra-rich combustion
(1:0 ¡  ¡ 1:5), partial oxidation (1:5 ¡  ¡ 2:5), and fuel
reformation ( ¿ 2:5). Furthermore, the driving factor for
these zones is kinetic rather than thermal.
Acknowledgements
The authors wish to acknowledge the National Science
Foundation through Grant number CTS-9812905. Also one
of the authors (JPB) held a Lincoln Fellowship during these
studies.
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