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International Journal of Hydrogen Energy 26 (2001) 265273
www.elsevier.com/locate/ijhydene
Eects of addition of electrolysis products on methane=airpremixed laminar combustion
C. Uykura, P.F. Henshawb; , D.S.-K. Tinga, R.M. Barrona
aMechanical Engineering, University of Windsor, 401 Sunset Avenue, Windsor, Ontario, Canada N9B 3P4bCivil and Environmental Engineering, University of Windsor, 401 Sunset Avenue, Windsor, Ontario, Canada N9B 3P4
Abstract
In this study, eects of the addition of small amounts of water electrolysis products on laminar premixed methane =air
ames have been investigated using chemical kinetic simulation methods. The CHEMKIN kinetic simulation package was
used with the GRI kinetic mechanism. Pollutant concentrations, ame speeds, temperature proles and lean ammability
limits of methane=air, methane=hydrogen=air and methane=hydrogen=oxygen=air systems were compared at dierent addition
percentages and equivalence ratios from 1.4 to the lean ammability limit. The addition of 10 20% hydrogen in the fuel
was found to have a small eect in improving ame speed and lean ammability limit properties. However, the addition of
oxygen and hydrogen in the same ratio as is found in water was shown to be benecial. Improvements in the ame speeds
of methane=air mixtures by the addition of 10% hydrogen and its associated oxygen were equivalent to the improvements
obtained by the addition of 20% hydrogen only. In near stoichiometric mixtures, the addition of oxygen substantially increased
the NOx concentrations, but for lean mixtures no increase in NOx was predicted. CO emissions were reduced when hydrogen
displaced carbon-containing fuels. ? 2001 International Association for Hydrogen Energy. Published by Elsevier Science
Ltd. All rights reserved.
Keywords: Water electrolysis products; Kinetic simulation; Hydrogen; Methane; Oxygen; CHEMKIN; GRI
1. Introduction
Natural gas, which is mainly composed of methane, oers
signicant economic [1] and environmental [2,3] advantages
over other fuels. Methane has lower emission levels com-
pared with other fuels because of its chemical formula (lower
carbon to hydrogen ratio) and utilizing it in leaner combus-tion can further reduce these levels. Leaner combustion of
methane may result in higher thermal eciency and reduced
emissions, especially of NOx . However, the low ignitibility
and lower ame speed of methane, which cause combustion
instabilities, excessive emissions and lower power output,
are the major impediments to achieving satisfactory results
with methane.
Corresponding author. Tel.: +01-519-253-4232 ext 2588; fax:
+01-519-971-3686.
E-mail address: [email protected] (P.F. Henshaw).
A practical solution to overcome the diculties with
methane is addition of more reactive fuels such as hydrogen.
There have been several investigations on the eects of the
addition of hydrogen into methane. It has been shown both
theoretically and experimentally that hydrogen addition
results in substantial enhancement in the ignitibility and
lean ammability limits of methane=air mixtures [417].Production of hydrogen by electrolysis of water may be
preferred because of the safety and cost considerations of
handling and storing hydrogen as a fuel additive [18,19].
The oxygen by-product of electrolysis can also be added
into the fuel=oxidizer mixture in order to improve combus-
tion properties. Practical applications of the addition of elec-
trolysis products into other fuels are already available in
the market. Although investigations concerning the utiliza-
tion of electrolysis products in practical devices such as IC
engines were performed in several studies [20,21], some
fundamental research is still needed to better understand
combustion kinetics of these mixtures without the compli-cations of operating a practical combustion device.
0360-3199/01/$ 20.00 ? 2001 International Association for Hydrogen Energy. Published by Elsevier Science Ltd. All rights reserved.
PII: S 0 3 6 0 - 3 1 9 9 ( 0 0 ) 0 0 0 6 8 - 9
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266 C. Uykur et al. / International Journal of Hydrogen Energy 26 (2001) 265273
In this study, the eects of the addition of small amounts
of hydrogen on methane=air combustion of premixed, lami-
nar, freely propagating, planar ames has been theoretically
investigated. In addition, since electrolysis of water may be
the source of hydrogen, the addition of hydrogen and oxy-
gen in the molar ratio H2 : O2 = 2 : 1 into a methane=airburner has been simulated.
2. The model
The numerical simulation was performed in order to pre-
dict adiabatic ame temperatures, pollutant concentrations
and ame speeds of laminar, premixed, freely propagating,
one-dimensional ames. The computational model used in
this study consists of the following components: PREMIX
[22], Sandias steady state, laminar, one-dimensional ame
code; TWOPNT [22], a boundary value problem solver;
a transport property preprocessor [22]; CHEMKIN-III [23],
a gas-phase interpreter which processes the chemical re-
action mechanism; and GRI 3.0 [24], a chemical reaction
mechanism for methane combustion.
PREMIX code which uses a hybrid time-integration=
Newton iteration technique to solve the steady-state com-
prehensive mass, species, and energy conservation equa-
tions was set up to simulate a freely propagating ame
with mixture-averaged formulas. An additional boundary
condition for mass ow rate, which is necessary for this
type of formulation, was obtained by xing the location of
the ame by specifying the temperature at one point. The
CHEMKIN package was modied to implement the GRImechanism by replacing its original reaction and transport
library with the GRI les. In this study, the GRI mechanism
version 3.0, which has 325 reactions and 53 species, was
used without any modication. The mechanism is described
extensively elsewhere [24].
The problem environment was dened by setting the ini-
tial and boundary conditions. The initial ow rate estimation
of the fuel=oxidizer mixture was set equal to 0:04 (g=cm2 s)
according to the published measurements of stoichiometric
methane=air ame speeds [25]. The pressure and tempera-
ture of the mixture were set at 1.0 atm and 298 K, respec-
tively. The additional boundary condition required for theow solution was supplied by xing the temperature point
for 400 K whose distance is calculated from the initial tem-
perature prole estimation by the software. Since it was
known from the previous studies [26] that the total reaction
zone of the premixed, laminar, freely propagating, stoichio-
metric methane=air ame is about 0.4 cm, the calculation
domain was started 2 cm before the ame region and the
total length of the calculation domain was chosen as 12 cm.
The initial temperature prole estimation, which is required
to start the iteration, was made according to the recent study
of VanMaaren et al. [26]. Results of the rst simulation step
were used as the temperature prole estimation for the next
step.
Table 1
Unreacted fueloxidizer composition of methane=air mixtures at
dierent equivalence ratios
O2 N2 CH4
1.5 0.1811 0.6831 0.13581.4 0.1827 0.6894 0.1279
1.3 0.1844 0.6957 0.1199
1.2 0.1861 0.7022 0.1117
1.1 0.1879 0.7088 0.1033
1 0.1896 0.7155 0.0948
0.9 0.1915 0.7224 0.0862
0.8 0.1933 0.7294 0.0773
0.7 0.1952 0.7365 0.0683
0.6 0.1971 0.7437 0.0591
0.5 0.1991 0.7511 0.0498
Table 2
Unreacted fueloxidizer composition of methane=air mixture with
the addition of 10% hydrogen by volume at dierent equivalence
ratios
O2 N2 CH4 H2
1.5 0.1791 0.6757 0.1307 0.0145
1.4 0.1808 0.6823 0.1232 0.0137
1.3 0.1826 0.6890 0.1155 0.0128
1.2 0.1844 0.6959 0.1077 0.0120
1.1 0.1863 0.7029 0.0997 0.0111
1 0.1882 0.7101 0.0916 0.0102
0.9 0.1901 0.7174 0.0832 0.0092
0.8 0.1921 0.7248 0.0748 0.0083
0.7 0.1941 0.7324 0.0661 0.00730.6 0.1962 0.7402 0.0573 0.0064
0.5 0.1983 0.7481 0.0482 0.0054
Numerical solutions were obtained for the following
mixtures: (1) pure methane=air, (2) 10% hydrogen + 90%
methane+air, (3) 20% hydrogen + 80% methane + air, (4)
10% hydrogen + oxygen (half as much as the hydrogen) +
90% methane + air (the initial concentrations of these mix-
tures can be found in Tables 14). Lean ammability
limits, nal temperature proles, ame speeds and species
concentration of these mixtures have been predicted fordierent equivalence ratios ().
3. Results and discussion
The solution algorithm was rst tested for accuracy by
comparing the ame speed at dierent equivalence ratios of
pure methane=air mixtures to published values. The ame
speed is dened as the speed, relative to and normal to the
ame front, with which unburned gas moves into the front
and is transformed to products under laminar ow condi-
tions [29]. In our study it was simply the velocity of gas
ow at the adiabatic boundary of the ame (ow velocity
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C. Uykur et al. / International Journal of Hydrogen Energy 26 (2001) 265273 267
Table 3
Unreacted fueloxidizer composition of methane=air mixture with
the addition of 20% hydrogen by volume at dierent equivalence
ratios
O2 N2 CH4 H2
1.5 0.1768 0.6672 0.1248 0.0312
1.4 0.1787 0.6742 0.1177 0.0294
1.3 0.1806 0.6813 0.1105 0.0276
1.2 0.1825 0.6886 0.1031 0.0258
1.1 0.1845 0.6961 0.0955 0.0239
1 0.1865 0.7038 0.0878 0.0219
0.95 0.1876 0.7076 0.0838 0.0210
0.9 0.1886 0.7116 0.0799 0.0200
0.85 0.1896 0.7155 0.0759 0.0190
0.8 0.1907 0.7195 0.0718 0.0179
0.7 0.1929 0.7277 0.0635 0.0159
0.6 0.1951 0.7361 0.0551 0.0138
0.5 0.1974 0.7446 0.0464 0.0116
Table 4
Unreacted fueloxidizer composition with addition of water elec-
trolysis products addition (10%) at dierent equivalence ratios
O2 N2 CH4 H2
1.5 0.1824 0.6696 0.1331 0.0147
1.4 0.1842 0.6763 0.1254 0.0139
1.3 0.1860 0.6831 0.1176 0.0130
1.2 0.1879 0.6900 0.1097 0.0121
1.1 0.1899 0.6971 0.1016 0.0112
1 0.1918 0.7043 0.0933 0.0103
0.9 0.1938 0.7117 0.0848 0.00940.8 0.1959 0.7193 0.0762 0.0084
0.7 0.1980 0.7270 0.0674 0.0074
0.6 0.2001 0.7348 0.0584 0.0064
0.5 0.2023 0.7429 0.0492 0.0054
at 0 distance). Values of laminar ame speed S0u , reported
in the literature have been characterized by substantial scat-
ter [25]. This scatter has been attributed to the fact that no
experiments can directly generate an ideal one-dimensional,
planar, adiabatic, steady, unstrained, laminar ame for which
S
0
u is dened. However, three recent and promising resultshave been chosen for comparison [26 28]. Fig. 1 illustrates
that the ame speed simulated by GRI is equal to or higher
than the measured results. This may be a consequence of
tuning the GRI mechanism using the experimental results
from earlier publications where the ame speed was mea-
sured to be higher [28]. However, as shown in Fig. 1, sim-
ulated results are in good agreement with Gu et al.s results
[28] in the lean side (up to equivalence ratio = 1:0). This
measurement set is approximately 10% lower than simula-
tion on the rich side of the curve. However, the rich side
simulations are in good agreement with Van Maarens data
[27], which gives lower than the simulated values for the
lean side. This can be explained by the stretch levels of dif-
Fig. 1. Simulated and measured [2628] laminar ame speeds of
methane=air mixtures.
Fig. 2. Eects of the hydrogen (10 and 20%) and hydrogen=oxygen
(10%) addition on laminar ame speeds at dierent equivalence
ratio methane=air mixtures.
ferent measuring methods and the strong relation between
the level of stretch and ame velocity for low Lewis number
mixtures. Lean methane mixtures are more stoichiometric at
the ame, leading to enhanced burning intensity [31].
The leanest combustible 1 methane=air mixture has been
predicted to be =0:55 with this solution method. This value
is also in good agreement with Zebatakiss [32] measured
value of = 0:54.
Flame speed predictions for methane=air combustion with
H2 and H2 + O2 addition can be seen in Fig. 2. Although
hydrogen has a ame speed seven times higher than
methane, adding 10% hydrogen increases the ame speed
of the mixture by only 8% at = 1:0. Adding 20% H2increases the ame speed by a maximum of 15% at the
stoichiometric condition, whereas a 13% higher levels
in ame speed were predicted with the addition of 10%
H2 + O2. The percentage increase in ame speed due to
1 Although the ammability limit is dened as the leanest fuel
oxidizer mixture ratio beyond which no ame will propagate [30],
in this study it is predicted as the leanest mixture that results in
temperature increase.
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268 C. Uykur et al. / International Journal of Hydrogen Energy 26 (2001) 265273
Fig. 3. Temperature prole of freely propagating premixed laminar
ames of dierent stoichiometric fuel mixtures.
Fig. 4. The eects of dierent additives on nal ame temperature
of freely propagating premixed laminar ame on dierent equiva-
lence ratios.
H2 or H2 + O2 addition is independent of the equivalence
ratio. The leanest ammable mixture for a freely prop-
agating laminar methane=air ame was predicted to be
= 0:55. This was improved to = 0:54 with the ad-
dition of 10% hydrogen. The addition of 20% hydrogen
produced no further improvement in lean ammability limit
( = 0:54). Results from the addition of 10% hydrogenwith accompanying oxygen into methane=air combustion
systems improved the lean ammability limit to = 0 :52.
The reason that the addition of oxygen leads to a further
increase in ame speed and lean ammability limit may be
explained by the increase in the oxygen and methane mole
fraction in the unburnt mixture compared with methane or
methane=hydrogen mixtures of the same equivalence ratio.
Temperature proles of dierent mixtures for the whole
ame area are illustrated in Fig. 3. Although all mixtures
appear to have similar temperature proles, the nal tem-
peratures (temperatures at the end of the computational
domain) vary for dierent mixtures as seen in Fig. 4.
Although hydrogen has a higher ame temperature com-
Fig. 5. The eects of dierent additives on nal carbon monoxide
concentrations.
Fig. 6. The eects of dierent additives on nal NO concentrations.
pared with methane, the ame temperature of the mix-
ture was increased by less than 1% even with the ad-
dition of 20% H2. The addition of oxygen into these
mixtures resulted in a further increase in nal ame
temperature of 1%. These increases are partially due
to the fact that the added oxygen resulted in less air
being added to maintain the same stoichiometry. The use
of oxygen instead of air at the same stoichiometry means
that less inert nitrogen is available to absorb heat in the
reaction, resulting in a higher temperature.
The carbon monoxide concentrations have been compared
for dierent mixtures in Fig. 5. The addition of hydrogencauses the overall carbon to hydrogen ratio of the mixture
to decrease (a pure hydrogen ame produces no CO). As a
result, CO concentrations for the hydrogen added mixtures
decreased. The decrease in CO as compared to methane was
not as great when oxygen was added to the unburnt mixture
due to the higher methane mole fraction. Dierences in CO
concentrations for all lean mixtures were negligibly small,
due to the low CO concentrations found at these equivalence
ratios.
The eects of hydrogen and oxygen addition on NO
concentrations for dierent equivalence ratio methane=air
mixtures are shown in Fig. 6. High temperatures and high
oxygen concentrations result in high NO formation rates
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Fig. 7. The eects of temperature and oxygen concentration on NO production rate for stoichiometric mixtures ( = 1) (a)
methane=air + hydrogen (b) methane=air + hydrogen + oxygen.
[29]. With hydrogen=methane mixtures, the slight increase in
temperature due to addition of H2 is compensated by the
decrease in oxygen concentration, leading to lower NO
concentrations in lean mixtures. The addition of oxygen
causes the mixture to have both an increase in oxygen con-centration and an increase in adiabatic ame temperature
leading to higher NO concentrations for those mixtures
near stoichiometry. However, for lean mixtures, dierences
in NO emissions are very small.
Figs. 7 and 8 illustrate the reasons for dierent emission
behaviors in dierent mixtures. In stoichiometric mixtures
( = 1), which have maximum total NO levels, an increase
in NO starts with an increase in temperature (0.05 cm)
but in the region that has higher oxygen levels (0.05 0.07
cm) no signicant NO production was observed because
the temperature was low. In Fig. 7, dNO=dt for hydro-
gen and hydrogen=oxygen added mixtures start to increase
as the temperatures are increased (0.07 cm). However,
dierences in NO production take place near the highest
temperature region (0.10 cm). Dierences in NO produc-
tion rate diverge, as the temperature levels are dierent. In
contrast, for lean mixtures (Fig. 8) NO production begins to
dier in the region that has relatively high oxygen concentra-tion dierences and relatively small temperature dierences
(0.7 cm). However, the NO production rates are similar in
regions where the temperature prole is dierent, such as
at 0.2 cm.
As can be seen in Fig. 9, the history of NO levels and
NO production rates are dierent for dierent equivalence
ratios. NO levels for lean mixtures increase up to a
maximum level within a certain distance but remain nearly
constant over the rest of the computational domain. But for
stoichiometric mixtures, increases in NO continue down-
stream till the end of the computational domain. To explain
the dierences in NO production, Fig. 10 is helpful. The
major reactions for NO production have been determined by
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270 C. Uykur et al. / International Journal of Hydrogen Energy 26 (2001) 265273
Fig. 8. The eects of temperature and oxygen concentration on NO production rate for lean mixtures ( = 0:6) (a) methane=air + hydrogen
(b) methane=air + hydrogen + oxygen.
reaction rate parameters and instantaneous concentrations
of reactants for all NO producing reactions. Not surpris-
ingly, the three most common reactions are the well-known
Zeldovich mechanism [29]:
O + N2 NO + N ; (1)
N + O2 NO + O ; (2)
N + OH NO + H : (3)
In dierent mixtures and at dierent equivalence ratios,
reactions responsible for the major NO production vary. For
lean mixtures (c and d), rates of all three reactions are sim-
ilar and reaction (2) has the maximum rate. This might be
the reason for oxygen concentration dependence of NO rates
for lean mixtures. For hydrogen added stoichiometric mix-
tures (a), reaction (3) has the maximum rate starting with the
maximum temperature and up to the end of the ame front.
However, for oxygen=hydrogen added stoichiometric mix-
tures (b), all three reactions have their maximum value at
dierent positions on the ame and have a similar non-zero
value downstream of the reacting front.Although NOx emissions are the total of NO and NO2,
as illustrated in Fig. 11, the nal NO2 concentrations for
all mixtures and all equivalence ratios were predicted to
be less than 1% of the nal NO concentrations. Also, NO2concentrations show similar trends as NO concentrations in
terms of H2 eects (cf. Fig. 11 with Fig. 6).
4. Conclusions
Hydrogen and oxygen have been proposed as additives
to methane-fueled combustion systems in order to improve
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Fig. 9. NO concentrations and NO production rates of lean and stoichiometric mixtures of methane=hydrogen=air andmethane=hydrogen=oxygen=air with respect to the ame distance.
pollutant emissions and thermal eciency. However, some
theoretical studies about kinetic behavior of these sys-
tems are essential to predict the possible benets and
to reduce drawbacks. In this study, the kinetics of hy-
drogen and oxygen addition eects on basic combustion
properties of methane laminar premixed ames were
investigated.
It has been found that the addition of 10 or 20% hydro-
gen to methane=air laminar premixed ames did not signi-
cantly improve the lean ammability limits. The maximum
increase in lean ammability limit was 2% which occurred
with 20% H2 addition. On the other hand, the addition of
10% hydrogen with oxygen in a H2 : O2 ratio of 2 : 1 resulted
in a 5% increase in lean ammability limit. The tempera-
ture proles and concentrations of pollutant species (NO,
NO2, and CO) for methane=air with 10 or 20% H2 mixtures
were predicted to be similar to the proles for methane =air
mixtures.
The addition of 10% H2 + O2 resulted in as much im-
provement in ame speed as the addition of 20% H2.
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Fig. 10. The eects of the dierent reactions on NO production for lean and stoichiometric mixtures.
Temperature proles of oxygen added mixtures were
predicted to be higher at all equivalence ratios. Car-
bon monoxide and NOx concentrations of oxygen
added mixtures are also higher than the 10 or 20% H2mixtures.
In summary, the addition of hydrogen and oxygen was
predicted to be more benecial than the addition of pure
hydrogen in terms of ame speed, temperature, lean
ammability limit, and CO concentrations. Increases in
NO concentrations were predicted to be higher with the
addition of hydrogen and oxygen. But it was shown
that these eects could be compensated by the exten-
sion in lean ammability limit. It is also clear that uti-
lizing hydrogen and oxygen as additives in practical
combustion systems may result in higher power outputs
because of the increase in fuel concentration in the mix-
ture compared with methane=air or methane=air + H2
mixtures.
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Fig. 11. The eects of dierent additives on nal NO2 concentra-
tions.
Acknowledgements
This project was partially sponsored by the Natural
Sciences and Engineering Research Council of Canada
(NSERC).
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