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Effect of Dilut ion by Nit rogen and/orCarbon Dioxide on Methane and Iso-Octane Air FlamesF. Halt er a , F. Foucher a , L. Landry a & C. Mounam-Rousselle aa

Instit ut PRISME, Universit D'Orleans, 45072 Orlans Cedex 2,France

Available online: 27 May 2009

To cite this art icle: F. Halter, F. Foucher, L. Landry & C. Mounam-Rousselle (2009): Effect of Dilut ionby Nit rogen and/ or Carbon Dioxide on Methane and Iso-Oct ane Air Flames, Combust ion Science andTechnology, 181:6, 813-827

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EFFECT OF DILUTION BY NITROGEN AND/OR CARBONDIOXIDE ON METHANE AND ISO-OCTANE AIR FLAMES

F. Halter, F. Foucher, L. Landry, and C. Mouna m-RousselleInstitut PRISME, Universite DOrleans, 45072 Orle ans Cedex 2, France

The impact of dilution on laminar burning speed of two different fuels (methane and isooc-tane) is studied. In the present study, three different diluents are used nitrogen, carbondioxide, and a mixture representative of exhaust gases issued from a stoichiometric combus-

tion of methane. Experimental results and PREMIX computations of the CHEMKIN package, using two different kinetic schemes, are presented and compared with literatureresults, when available. Initial pressure and temperature conditions are respectively0.1MPa and 300 K. For both fuels, a larger decrease of the laminar burning speed isobtained for carbon dioxide dilution than for nitrogen dilution. This observation is directlylinked to the increase in heat capacity of the dilution gas but also to the carbon dioxidedissociation, even if the heat capacity effect seems to be predominant.

Keywords : Dilution; Laminar burning speed

INTRODUCTION

Exhaust gases recirculation presents an interesting potential to reduce NO xemissions. Indeed, the reintroduction of burnt gases in the fresh gases dilutes themixture and induces a combustion temperature diminution, one of the main criteriaof NO x formation. However, this dilution also affects the reactivity of the ame andthus engine stability. In spark-ignition engines, the turbulent propagation speed of the ame front is a key parameter in the engine stability. With the introduction of the amelet concept (Clavin, 1985), the turbulent ame is viewed as an ensembleof laminar ame elements. Locally, the ame element displacement is piloted bothby aerodynamic motions and by the laminar burning speed.

The present study aims at characterizing the dilution effect on laminar burningspeed for two different fuels: methane and iso-octane. Methane is the main com-pound of natural gas, which is commonly used in SI engines. Iso-octane is one of many different compounds of gasoline; this choice was based on the coherence inoctane number but also on the close burning speed of iso-octane and gasoline(Jerzembeck et al., 2009). Moreover, only few results are available in the literaturefor diluted iso-octane =air ames (Huang et al., 2004; Ryan & Lestz, 1980), even if some results can be found for other fuels such as methane (Burke & Van Tiggelen,

Received 3 February 2008; revised 30 April 2008; accepted 4 March 2009.Address correspondence to F. Halter, Institut PRISME, Universite DOrleans, 8 Rue Le onard de

Viinci 45072 Orleans cedex 2, France. E-mail: [email protected]

Combust. Sci. and Tech. , 181: 813827, 2009Copyright # Taylor & Francis Group, LLCISSN: 0010-2202 print =1563-521X onlineDOI: 10.1080/00102200902864662

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1965; Dong et al., 2002; Elia et al., 2001; Liao et al., 2004; Ponnusamy et al., 2005;Stone et al., 1998; Tanoue, 2003), propane (Zhao et al., 2004), n-decane (Zhao et al.,2005), n-butane (Huang et al., 2002), methanol (Zhang et al., 2008), or for a realgasoline (Zhao et al., 2003).

In the present paper, the impact of three different diluents (N 2 , CO 2 , and amixture of both) is studied on stoichiometric methane and iso-octane air ames.Water is not considered in the different EGR compositions for this present work.Indeed, the initial temperature (300 K) is too low to allow a complete vaporizationof water; based on vapor pressure evaluation (Yaws, 1999), dilution level can onlybe of 3% in volume at these thermo-dynamical conditions. Dlugogorski et al.(1998) have evaluated the inuence of water vapor on natural gas laminar burningspeeds by working with higher temperatures (i.e., 373 and 423 K). Therefore, for thiswork, the water volume is considered in the CO 2 content. This approximation ismotivated by their close heat capacities: 33 J =mol K for H 2 O and 37 J =mol K for

CO 2 at 0.1 MPa and 300 K.All experimental and numerical results are presented and compared withresults from literature.

EXPERIMENTAL SETUP

The experimental setup used is composed of a stainless steel cylindricalcombustion chamber of 24 liters, two tungsten electrodes (dia. 2 mm) linked to a highvoltage source, an Ar-Ion laser, and a high-speed camera. Optical accesses into thechamber are provided by four windows. The combustible mixture is prepareddirectly in the chamber by adding the fuels (methane or iso-octane) and the air atappropriate partial pressures to reach the total initial pressure (0.1 MPa). For experi-ments with iso-octane, the correct liquid quantity of fuel is weighted with a high-precision balance (four signicant digits after the gram). The adequate iso-octanequantity is placed in a tube linked to the injector. This tube is then pressurized withcompressed air. Fuel quantity is fully injected in the chamber by using a solenoidinjector. To ensure the complete injection, some air is injected at the end of the injec-tion. In the same way, the chamber is lled with the balance of the mixture (air anddiluents). The injection timing (frequency and gate) is adjusted to nish the injectionprocess just before the lling process. To facilitate the vaporization, a fan is locatedinside the chamber. The fan mixes all the gases for almost ve minutes. Finally,

the mixture is left at rest to avoid any perturbation during the ame propaga-tion. The saturated vapor pressure of iso-octane at 300K is 5.86 kPa. With the limitof vaporization, we could study gaseous stoichiometric mixture of iso-octane =air upto 0.3MPa. At atmospheric pressure, the quantity of iso-octane injected is threetimes lower than the saturated vapor pressure. In these conditions, the quantity of fuel injected should be fully vaporized. To ensure the mixture, fresh gases wereanalyzed using gas chromatography.

The visualization of the ame is obtained by the classical shadowgraphymethod. The parallel light is created by two plano-convex lenses (25 mm and1000mm focal lengths, respectively). The shadowgraphs are recorded using ahigh-speed video camera (Photron APX) operating at 6000 frames per second withan exposure time of 20 ms. A schematic view of the system is presented in Figure 1.

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The temporal evolution of the expanding spherical ame is imaged andanalyzed. Fundamental laminar burning velocities are then obtained, taking intoaccount both the effects of the expansion factor and the stretch (Bradley et al.,1998; Halter et al., 2005). All experimental values of laminar burning speed reportedin this paper are the average of three identical experiments.

Laminar Burning Speed Extraction

The evolution of the ame radius is obtained by extrapolating the ame front

to the luminous front. With this method, the propagation speed of the fresh gases isobtained. When dilution percentage is elevated, the ame propagation is affected bynatural convection, as illustrated in Figure 2. In these conditions, only the upper partof the ame is studied, and the ame center is readjusted for each time step.

Figure 2 Flame picture for a N 2 dilution of 24% (CH 4 -air ames, P 0.1MPa, T 300 K, U 1).

Figure 1 Schematic view of the system.

EFFECT OF DILUTION ON METHANE AND ISO-OCTANE AIR FLAMES 815

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An example of ame front radius (R f ) temporal evolution for a stoichiometriciso-octane =air mixture (P ini 0.1 MPa T ini 300K) is presented in Figure 3. Theame radius evolution is obtained from the derivation of the temporal radiusevolution. The stretched propagation speed is then obtained by a derivation of thispolynomial:

V S dR f

dt

1

The propagation speed for a stoichiometric iso-octane =air mixture (P ini 0.1 MPa T ini 300K) is presented in Figure 4.

Figure 3 Evolution of the ame radius as a function of time, iso-C 8 H 18 =air mixture.

Figure 4 Evolution of the propagation speed as a function of time, iso-C 8 H 18 =air mixture (P 0.1MPa,T 300K, U 1).


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The relative rate change of the ame area constitutes the ame stretch(Williams, 1985):

j

1A

dAdt ; 2

with A the ame surface and t the time.Karlovitz et al. (1953) were the rst to introduce the concept of stretch

rate. Signicant effects of ame stretch on laminar burning speed can be observedfor values of R f (ame radius) that are largely greater than the characteristic amethickness (Fristom, 1965; Palm-Leis & Strehlow, 1969). In the case of a sphericalexpanding laminar ame, the total stretch acting on the ame is dened as(Law, 1988):

j 2V S

R f 3

The relation between laminar burning speed and ame stretch was based on an ear-lier proposal of Markstein (1964). For moderate curvature and strain rates, we canconsider the normal ame speed varies linearly with the ame stretch. This propertyis used in the treatment as shown in Figure 5. The unstretched propagation speed isobtained via a zero stretch extrapolation. During this study, we will use the denitionsuggested by Clavin (1985):

V S V 0S L j 4

where V 0S is the value for an unstretched (plane) ame, and L is the Markstein length,a measure of the response of the ame to stretch. The Markstein length can be eitherpositive or negative depending on the properties of the reactant mixture.

Figure 5 Evolution of the propagation speed as a function of stretch, iso-C 8 H 18 =air mixture (P 0.1MPa,T 300 K, U 1). The dashed red line correspondens to the zero stretch extrapolation.


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The unstretched burning speed ( S 0L ) is deduced from V 0S using (Strehlow et al.,1978):

V 0S S 0L

q u

q b 5

where q u and q b are respectively the unburned and the burned gas density. Fresh andburnt gases are supposed to behave as perfect gases. The combustion process isassumed to be isobaric. As a consequence, the density ratio is related to the ratioof the burned to unburned gas temperature. Burnt gas temperature was evaluatedfrom adiabatic calculations.

For our experiments, measurements of ame radius were limited to 0.06 m. Forsuch conditions, the volume of burned gas was less than 0.5% of the total chambervolume. Within this region, one can consider that the total chamber pressure is con-

stant. The magnication of the system leads to a spatial resolution of 145 mm=pixels.Each diameter is determined with an accuracy of 1 pixel. To avoid the effect of energy deposition, the minimum radius under studied is of 0.005 m. Thus, the maxi-mal error made on the radius measurement will be of 6%. At the end of the measure-ment (for a radius of 0.03 m), the error is of 1%.

RESULTS

Methane/Air Flames

The rst step was to evaluate the evolution of the laminar burning speedfor different equivalence ratio conditions. Correct agreement was obtained withliterature (Halter et al., 2005). Then, dilution impact was tested on stoichiometricCH 4 =air ames.

Several authors started to evaluate the potential of diluted methane =air ames(Elia et al., 2001; Liao et al., 2004; Ponnusamy et al., 2005; Stone et al., 1998). Stoneet al. (1998) obtained laminar burning speed of methane =air=diluents mixtures forvariation in unburnt gas temperature (within 293 to 454K) and pressures (withinthe range of 0.05 to 1.04MPa) under microgravity conditions. Carbon dioxide, nitro-gen, and a 15% carbon dioxide =85% nitrogen mixture were used as diluents. Thecomparison with their results for N 2 and CO 2 dilution is biased by the fact that they

consider only a dilution of the fuel and not of the global mixture (air fuel), whichmodify the global equivalence ratio. In our case, the equivalence ratio is kept con-stant and equal to stoichiometry.

Nitrogen and carbon dioxide addition effects on CH 4 =air ames are reportedin Figure 6. Experiments are represented by symbols and computations using thePREMIX code of the CHEMKIN package, with the GRIMech 3.0 (Smith et al.)as kinetic scheme designated by solid lines. PREMIX computations were performedusing a freely propagating ame conguration. The computational domain was xedfrom 0 to 12. The mesh adaptive criteria were taken equal to 0.2, both for curvatureand gradient. The number of initial mesh points was xed to 20.

One can conclude that the laminar burning speed decreases as the dilution rateincreases. This decrease is more important for CO 2 than for N 2 , which is consistent


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with literature. A very good agreement between experiments and computations isobtained for both dilutions.

The decrease of the laminar burning speed could be due to two phenomena: thedifference of heat capacity for the diluent gases and the dissociation of carbon diox-ide. In order to estimate their relative impact, we performed simulations by introdu-

cing a new molecule (F-CO 2 , for False CO2 ) that possesses the thermal andtransport characteristics of carbon dioxide but is chemically inactive. This moleculedoes not react and its concentration remains constant during the entire combustionprocess. In order to know the relative importance of CO 2 dissociation, CO 2 isreplaced in the new computations by F-CO 2 . Numerical results obtained with thisnew diluent are reported in Figure 7. We observe that laminar burning velocitiescorresponding to F-CO 2 are located between those corresponding to nitrogen andcarbon dioxide dilution. As a consequence, the dissociation effect is non-negligible.As an example, if we consider a dilution rate of 5%, we obtain a laminar burningspeed of 0.32 m=s for a nitrogen dilution. If we consider a carbon dioxide dilution,the laminar burning speed is decreases to 0.26 m =s. Now, if we consider a dilutionwith the non-reacting carbon dioxide (F-CO 2 ), the laminar burning speed reachesthe value of 0.29 m =s. This laminar burning speed reduction, compared to the valueobtained for a nitrogen dilution, can be only linked to the increase of the heatcapacity. As a consequence, the inuence of heat capacity can be simply evaluatedby S

0L N 2S

0L FCO 2

S 0L N 2S 0L CO 2

, with S 0L the laminar burning speed. In Figure 8, we plotted therelative contributions of heat capacity increase and carbon dioxide dissociation inthe diminution of the laminar burning speed (compared to a nitrogen dilution).Flame speed reduction for a carbon dioxide dilution of 5% is due equally to carbondissociation and to the higher heat capacity of carbon dioxide. However, the effect of carbon dioxide dissociation is less important when the dilution rate is increased: theglobal temperature is lower and does not support carbon dioxide dissociation.

Figure 6 Effect of N 2 and CO 2 dilution on the laminar burning speed of stoichiometric CH 4 =air ames(P 0.1MPa, T 300 K, U 1). Symbols represent experimental data. Dashed lines represent PREMIXcomputations using the GRIMech 3.0.


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We will now focus on a more representative mixture of exhaust gases. Elia et al.(2001) investigated experimentally the laminar burning velocities of methane =airames with the addition of a mixture of 86% N 2 and 14% CO 2 , in order to simulatethe effect of residual gases from exhaust gas recirculation. They used a thermodyn-amic model to evaluate the laminar burning speed from a pressure-time history of the combustion process. Liao et al. (2004) achieved an explicit formula of laminarburning velocities for dilute mixtures (88% N 2 12% CO 2 ). In Ponnusamy et al.(2005), the EGR was simulated by a mixture of 81.5% N 2 and 18.5% CO 2 .

By considering water in the CO 2 content, the EGR is simulated by a mixture of 71.6% N 2 and 28.4% CO 2 (instead of 71.6% N 2 , 9.5% CO 2 , and 18.9% of H 2 O). Ourresults and computations are presented in Figure 9.

Figure 8 Contribution of the heat capacity and of the dissociation of carbon dioxide on the decrease of laminar burning velocities (CH 4 -air ames, P 0.1MPa, T 300 K, U 1).

Figure 7 Calculated laminar burning velocities for CO 2 , F-CO 2 (non-reacting CO 2 ), and N 2 of stoichio-metric CH 4 =air ames (P 0.1MPa, T 300 K, U 1).


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As expected, we observe a decrease of the laminar burning speed when EGRis added. Our results exhibit a good agreement with results from other authors, evenif the mixture compositions are slightly different. The laminar burning speed is not assensitive to the mixture composition. Results from computations are also in goodagreement with our experimental results. As a conclusion, GRI Mech 3.0 is correctlyvalidated for methane =dilution =air mixtures (for T 300 K and P 0.1MPa).

Markstein lengths, as determined from Eq. (4), are displayed in Figure 10 formethane =air ames (P 0.1 MPa, T 300K, U 1) diluted with nitrogen. First,

Markstein lengths are positive, which denotes stable ames. Indeed, the laminarburning velocity decreases with increasing stretch. Flame elements that are concavetoward the combustion products have a negative stretch (i.e., become smaller), andthe ame is then stable. As the dilution rate increases, so does the Markstein length.

Figure 9 Effect of EGR (71.6% N 2 and 28.4% CO 2 ) dilution on the laminar burning speed of stoichio-

metric CH 4 =air ames (P 0.1MPa, T 300 K,U

1).

Figure 10 Effect of nitrogen dilution on the Markstein length for stoichiometric CH 4 =air ames(P 0.1MPa, T 300K, U 1).


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The inuence of stretch on ame increases with the percentage of dilution for stoe-chiometric methane =air ames. This was compared to the evolution observed whenleaning the mixture. Rozenchan et al. (2002) and Gu et al. (2000) pointed out adecrease of the Markstein length when the equivalence ratio is moved from stoechio-metry to lean mixtures (i.e., when air is added). This difference in Markstein lengthevolution when nitrogen or air is added to a methane =air mixture could nd its expla-nation in the different Lewis number evolution. Indeed, for a methane =air mixture,the Lewis number is reduced when diluted with nitrogen (Tanoue, 2003), whereas itis increased when diluted with air (Clarke, 2002; Tanoue, 2003). As in the presentwork, Markstein length increase was observed for a nitrogen dilution by severalauthors but for different fuelsnatural gas with small amounts of hydrogen (Miaoet al., 2009), propane (Zhao et al., 2004) and methanol (Zhang et al., 2008).

Results for Iso-Octane

Laminar burning velocities obtained for different equivalence ratios and resultsissued from other authors (Davis & Law, 1998; Huang et al., 2002; Metghalchi &Keck, 1982) are presented in Figure 11. Liao et al. (2004) and Metghalchi and Keck(1982) performed their experiments in a constant volume bomb. Davis et al. used acounterow thin ame conguration. We used the reduced mechanism of Hasse et al.(2000) in our computations. Good agreement is obtained with data available inliterature and with PREMIX computations.

Experimental results and numerical simulations (with the mechanism of Hasseet al., 2000) of diluted stoichiometric mixtures are presented in Figure 12. The effectsof nitrogen, carbon dioxide, and simulated EGR dilutions on laminar burning velo-cities are investigated. The experimental limit is reached for a non-propagation of theame front. A larger decrease of the laminar burning velocities is observed whencarbon dioxide is added (compared to nitrogen dilution). Values obtained for asimulated EGR (71.6% N 2 and 28.4% CO 2 ) dilution are located between nitrogen

Figure 11 Laminar burning speed of iso-C 8 H 18 =air ames for different equivalence ratios (P 0.1MPa,T 300K).


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whatever the nature of dilution, Markstein lengths are increased. The smaller theMarkstein length is, the less important the inuence of stretch on laminar burningvelocity is. As a consequence, the inuence of stretch on ame increases with thepercentage of dilution. The ame is globally less stable.

The evolutions of burning rate (i.e., q u S 0L with q u , the fresh gases density)have been plotted in Figure 15 for different dilution rates. The burning rate corre-

sponds to the global reactivity of the mixture. Evolutions are almost similar to thoseobserved for laminar burning velocities because of quasi-similarities of the differentmixtures.

Figure 14 Markstein length for different dilution conditions, iso-C 8 H 18 -air ames (P 0.1MPa,T 300K, U 1).

Figure 15 Reaction rates for different dilution conditions, iso-C 8 H 18 -air ames (P 0.1MPa, T 300K,U 1).


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CONCLUSION

The present work aims at characterizing the effect of dilution on the laminarburning speed of CH 4 =air and i-C 8 H 18 =air ames. Three different diluents are used:

nitrogen, carbon dioxide, and a mixture of both (71.6% N 2 and 28.4% CO 2 ). Experi-mental results and PREMIX computations are presented and compared with litera-ture results, when available. Pressure and temperature conditions are respectively0.1 MPa and 300 K.

For methane =air ames, our computations were done by using the GRI Mech3.0. As expected, the laminar burning speed decreases when the mixture is diluted.Computations with PREMIX are in very good agreement with our results. Forour initial thermodynamics conditions, the validity of the GRI Mech 3.0 is testedwith success. Compared to nitrogen dilution, carbon dioxide dilution induces a lar-ger decrease of the laminar burning speed. This is linked to the increase in heatcapacity and also to carbon dioxide dissociation. The effect of carbon dioxide dis-sociation becomes less important when dilution level is increased, because the ametemperature is largely affected by dilution.

One limit of these experiments is reached with high dilution levels. Indeed,convection effects are no more negligible and affect largely the ame propagation.A solution to this problem could be to perform experiments under microgravity con-ditions, as done by Stone (1998). However, their analysis is based on the pressureevolution (according to Dahoe and de Goey [2003], this method is not the mostsuitable one), and their microgravity is created thanks to a drop of 0.3 m (whichis limited).

Results for iso-octane =air mixtures are in good agreement with literature and

numerical simulations. The dilution by carbon dioxide induces a larger decrease thana dilution by nitrogen and also by a mixture representative of exhaust gases (71.6%N 2 and 28.4% CO 2 ). This is due to the increase of heat capacity and carbon dioxidedissociation. By considering the global reaction rate, a decrease is still observed withthe increase of the dilution rate.

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