International Journal of Hydrogen Energy 26 (2001) 265273

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E ects of addition of electrolysis products on methane= air premixed laminar combustion

C. Uykur a , P.F. Henshawb ; , D.S.-K. Tinga , R.M. Barrona
b Civil a Mechanical

Engineering, University of Windsor, 401 Sunset Avenue, Windsor, Ontario, Canada N9B 3P4 and Environmental Engineering, University of Windsor, 401 Sunset Avenue, Windsor, Ontario, Canada N9B 3P4

Abstract In this study, e ects 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 di erent 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 e ect 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, o ers signicant economic [1] and environmental [2,3] advantages over other fuels. Methane has lower emission levels compared with other fuels because of its chemical formula (lower carbon to hydrogen ratio) and utilizing it in leaner combustion can further reduce these levels. Leaner combustion of methane may result in higher thermal e ciency 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: henshaw@uwindsor.ca (P.F. Henshaw).

A practical solution to overcome the di culties with methane is addition of more reactive fuels such as hydrogen. There have been several investigations on the e ects 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 [4 17]. 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 combustion properties. Practical applications of the addition of electrolysis products into other fuels are already available in the market. Although investigations concerning the utilization 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 complications 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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C. Uykur et al. / International Journal of Hydrogen Energy 26 (2001) 265273 Table 1 Unreacted fueloxidizer composition of methane= air mixtures at di erent equivalence ratios O2 1.5 1.4 1.3 1.2 1.1 1 0.9 0.8 0.7 0.6 0.5 0.1811 0.1827 0.1844 0.1861 0.1879 0.1896 0.1915 0.1933 0.1952 0.1971 0.1991 N2 0.6831 0.6894 0.6957 0.7022 0.7088 0.7155 0.7224 0.7294 0.7365 0.7437 0.7511 CH4 0.1358 0.1279 0.1199 0.1117 0.1033 0.0948 0.0862 0.0773 0.0683 0.0591 0.0498

In this study, the e ects of the addition of small amounts of hydrogen on methane= air combustion of premixed, laminar, 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 oxygen in the molar ratio H2 : O2 = 2 : 1 into a methane= air burner has been simulated. 2. The model The numerical simulation was performed in order to predict 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 reaction 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 comprehensive mass, species, and energy conservation equations 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 GRI mechanism 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 initial 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 temperature of the mixture were set at 1.0 atm and 298 K, respectively. The additional boundary condition required for the ow solution was supplied by xing the temperature point for 400 K whose distance is calculated from the initial temperature 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, stoichiometric 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 2 Unreacted fueloxidizer composition of methane= air mixture with the addition of 10% hydrogen by volume at di erent equivalence ratios O2 1.5 1.4 1.3 1.2 1.1 1 0.9 0.8 0.7 0.6 0.5 0.1791 0.1808 0.1826 0.1844 0.1863 0.1882 0.1901 0.1921 0.1941 0.1962 0.1983 N2 0.6757 0.6823 0.6890 0.6959 0.7029 0.7101 0.7174 0.7248 0.7324 0.7402 0.7481 CH4 0.1307 0.1232 0.1155 0.1077 0.0997 0.0916 0.0832 0.0748 0.0661 0.0573 0.0482 H2 0.0145 0.0137 0.0128 0.0120 0.0111 0.0102 0.0092 0.0083 0.0073 0.0064 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 mixtures can be found in Tables 1 4). Lean ammability limits, nal temperature proles, ame speeds and species concentration of these mixtures have been predicted for di erent equivalence ratios ( ). 3. Results and discussion The solution algorithm was rst tested for accuracy by comparing the ame speed at di erent 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 conditions [29]. In our study it was simply the velocity of gas ow at the adiabatic boundary of the ame ( ow velocity

C. Uykur et al. / International Journal of Hydrogen Energy 26 (2001) 265273 Table 3 Unreacted fueloxidizer composition of methane= air mixture with the addition of 20% hydrogen by volume at di erent equivalence ratios O2 1.5 1.4 1.3 1.2 1.1 1 0.95 0.9 0.85 0.8 0.7 0.6 0.5 0.1768 0.1787 0.1806 0.1825 0.1845 0.1865 0.1876 0.1886 0.1896 0.1907 0.1929 0.1951 0.1974 N2 0.6672 0.6742 0.6813 0.6886 0.6961 0.7038 0.7076 0.7116 0.7155 0.7195 0.7277 0.7361 0.7446 CH4 0.1248 0.1177 0.1105 0.1031 0.0955 0.0878 0.0838 0.0799 0.0759 0.0718 0.0635 0.0551 0.0464 H2 0.0312 0.0294 0.0276 0.0258 0.0239 0.0219 0.0210 0.0200 0.0190 0.0179 0.0159 0.0138 0.0116

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Fig. 1. Simulated and measured [26 28] laminar ame speeds of methane= air mixtures.

Table 4 Unreacted fueloxidizer composition with addition of water electrolysis products addition (10%) at di erent equivalence ratios O2 1.5 1.4 1.3 1.2 1.1 1 0.9 0.8 0.7 0.6 0.5 0.1824 0.1842 0.1860 0.1879 0.1899 0.1918 0.1938 0.1959 0.1980 0.2001 0.2023 N2 0.6696 0.6763 0.6831 0.6900 0.6971 0.7043 0.7117 0.7193 0.7270 0.7348 0.7429 CH4 0.1331 0.1254 0.1176 0.1097 0.1016 0.0933 0.0848 0.0762 0.0674 0.0584 0.0492 H2 0.0147 0.0139 0.0130 0.0121 0.0112 0.0103 0.0094 0.0084 0.0074 0.0064 0.0054

Fig. 2. E ects of the hydrogen (10 and 20%) and hydrogen= oxygen (10%) addition on laminar ame speeds at di erent equivalence ratio methane= air mixtures.

0 at 0 distance). Values of laminar ame speed Su , reported in the literature have been characterized by substantial scatter [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 0 Su is dened. However, three recent and promising results have 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 measured to be higher [28]. However, as shown in Fig. 1, simulated 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 simulation 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-

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% H2 increases 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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Fig. 5. The e ects of di erent additives on nal carbon monoxide concentrations. Fig. 3. Temperature prole of freely propagating premixed laminar ames of di erent stoichiometric fuel mixtures.

Fig. 6. The e ects of di erent additives on nal NO concentrations.

Fig. 4. The e ects of di erent additives on nal ame temperature of freely propagating premixed laminar ame on di erent equivalence ratios.

H2 or H2 + O2 addition is independent of the equivalence ratio. The leanest ammable mixture for a freely propagating laminar methane= air ame was predicted to be = 0:55. This was improved to = 0:54 with the addition of 10% hydrogen. The addition of 20% hydrogen produced no further improvement in lean ammability limit ( = 0:54). Results from the addition of 10% hydrogen with 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 di erent mixtures for the whole ame area are illustrated in Fig. 3. Although all mixtures appear to have similar temperature proles, the nal temperatures (temperatures at the end of the computational domain) vary for di erent mixtures as seen in Fig. 4. Although hydrogen has a higher ame temperature com-

pared with methane, the ame temperature of the mixture was increased by less than 1% even with the addition 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 di erent mixtures in Fig. 5. The addition of hydrogen causes 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. Di erences in CO concentrations for all lean mixtures were negligibly small, due to the low CO concentrations found at these equivalence ratios. The e ects of hydrogen and oxygen addition on NO concentrations for di erent 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 e ects of temperature and oxygen concentration on NO production rate for stoichiometric mixtures ( methane= air + hydrogen (b) methane= air + hydrogen + oxygen.

= 1) (a)

[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 concentration and an increase in adiabatic ame temperature leading to higher NO concentrations for those mixtures near stoichiometry. However, for lean mixtures, di erences in NO emissions are very small. Figs. 7 and 8 illustrate the reasons for di erent emission behaviors in di erent 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= d t for hydrogen and hydrogen= oxygen added mixtures start to increase as the temperatures are increased (0.07 cm). However,

di erences in NO production take place near the highest temperature region (0.10 cm). Di erences in NO production rate diverge, as the temperature levels are di erent. In contrast, for lean mixtures (Fig. 8) NO production begins to di er in the region that has relatively high oxygen concentration di erences and relatively small temperature di erences (0.7 cm). However, the NO production rates are similar in regions where the temperature prole is di erent, such as at 0.2 cm. As can be seen in Fig. 9, the history of NO levels and NO production rates are di erent for di erent 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 downstream till the end of the computational domain. To explain the di erences in NO production, Fig. 10 is helpful. The major reactions for NO production have been determined by

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Fig. 8. The e ects 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 surprisingly, the three most common reactions are the well-known Zeldovich mechanism [29]: O + N2 N + O2 N + OH NO + N; NO + O; NO + H: (1) (2) (3)

In di erent mixtures and at di erent equivalence ratios, reactions responsible for the major NO production vary. For lean mixtures (c and d), rates of all three reactions are similar 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 mixtures (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 mixtures (b), all three reactions have their maximum value at di erent 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, NO2 concentrations show similar trends as NO concentrations in terms of H2 e ects (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 and methane= hydrogen= oxygen= air with respect to the ame distance.

pollutant emissions and thermal e ciency. However, some theoretical studies about kinetic behavior of these systems are essential to predict the possible benets and to reduce drawbacks. In this study, the kinetics of hydrogen and oxygen addition e ects on basic combustion properties of methane laminar premixed ames were investigated. It has been found that the addition of 10 or 20% hydrogen to methane= air laminar premixed ames did not signicantly 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 temperature 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 improvement in ame speed as the addition of 20% H2 .

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Fig. 10. The e ects of the di erent reactions on NO production for lean and stoichiometric mixtures.

Temperature proles of oxygen added mixtures were predicted to be higher at all equivalence ratios. Carbon monoxide and NOx concentrations of oxygen added mixtures are also higher than the 10 or 20% H2 mixtures. 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 e ects could be compensated by the extension in lean ammability limit. It is also clear that utilizing hydrogen and oxygen as additives in practical combustion systems may result in higher power outputs because of the increase in fuel concentration in the mixture compared with methane= air or methane= air + H2 mixtures.

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[14] [15]

[16] [17] Fig. 11. The e ects of di erent additives on nal NO2 concentrations. [18] [19]

Acknowledgements This project was partially sponsored by the Natural Sciences and Engineering Research Council of Canada (NSERC). References
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