Flame Studies of Small Hydrocarbons and Oxygenated Fuels
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1 Flame Studies of Small Hydrocarbons and Oxygenated Fuels Peter Veloo, Yang L. Wang, Okjoo Park, Qiayo Feng, Aydin Jalali, Roe Burrell, Adam Fincham, Charles K. Westbrook, Fokion N. Egolfopoulos Department of Aerospace and Mechanical Engineering University of Southern California SECOND ANNUAL CONFERENCE Combustion Energy Frontier Research Center (CEFRC) August 17-19, 2011 Princeton, New Jersey DoE Grant: DE-SC Period of performance: 8/1/09 7/31/14 Technical Monitor: Dr. Wade Sisk
2 General Objectives 1. To determine archival fundamental flame data for oxygenated fuels that are of relevance to transportation: Flame propagation Flame ignition Flame extinction NO x concentrations Soot volume fractions 2. To model the experimental data using detailed description of chemical kinetics and molecular transport. 3. To provide insight into the effects of the location and type of the O-containing functional group as a function of the carbon number on the fuel oxidation in flame environments. 4. To advance new/alterative approaches to study fundamental flame phenomena under various conditions, including extreme ones.
3 General Parameter Space Fuel chemical classifications: DME (target) C 1 -C 4 alcohols (target) C 1 -C 11 methyl & ethyl (saturated & unsaturated) esters (target) aldehydes (supporting) ketones (supporting) H 2 and CO (supporting) C 1 -C 4 n-alkanes and n-alkenes (supporting) Flame configurations: premixed non-premixed Thermodynamic conditions: wide range of reactant and inert compositions initial reactant temperatures:» ambient to 1200 K pressures:» atm (present capabilities)» > 30 atm (projected)
4 Counterflow flames Experimental Approach (1) Atmospheric rig for propagation/ extinction studies Atmospheric rig for soot/no x studies High-pressure rig for ignition studies, with transient plasma capabilities (newly established) High-pressure rig for propagation/ extinction studies High-pressure chamber for soot/no x studies with transient plasma capabilities (under development) o Diagnostics: Digital Particle Image Velocimetry (DPIV) Lase Doppler Velocimetry (LDV) Thermocouples Chemiluminescence (NO x ) Laser extinction (soot volume fractions)
5 Experimental Approach (2) Spherically expanding flames. Intention: NOT to duplicate the Princeton efforts! o Diagnostics: Shadowgraph (established) Digital Particle Image Velocimetry (DPIV) (under development) Constant volume chamber for ignition/propagation studies, with transient plasma capabilities (newly established)
6 Modeling Approach: Algorithms and Implementation o Use of CHEMKIN-based codes Steady 1-D flames Unsteady 1-D flames (Y H )max o Proper description of turning-point behavior 1/K, s o Mathematically rigorous determination of logarithmic sensitivity coefficients: (lny)/ (lnx) Y: laminar flame speed / extinction strain rate / ignition temperature X: A-factor / D i-n2 o All numerical results have been produced by solutions that: Were properly converged, i.e. in highly resolved grids Included the effects of thermal radiation and Soret Included full multi-component transport formulation Included all pertinent experimental boundary conditions
7 Modeling Approach: Kinetic Models o Notable differences in fuel kinetics among various models o Notable differences in C 0 -C 4 kinetics among various models o Most models tested in their entirety (hard to distinguish the source of a problem) o All fuel kinetics were superimposed on the USC Mech II and/or JetSurf models: distinguish between fuel and foundation kinetics assess in the most meaningful way the effects of fuel molecular structure on a variety of fundamental flame properties resulting (combined) models are merely analysis tools and NOT for dissemination
8 Specific Fuels Alcohol-related: Methanol Ethanol Propanol isomers Butanol isomers Ketones Aldehydes Corresponding n-alkanes C 0 -C 4 hydrocarbons Biodiesel-related: C 1 -C 4, C 9 -C 11 esters: Methyl Ethyl Saturated Unsaturated Corresponding n-alkanes Diesel surrogates C 0 -C 4 hydrocarbons
9 Progress During Year 1 1. Propagation and extinction of flames of neat and mixtures of H 2 /CO/C 1-4 hydrocarbons» (33 rd Combustion Symposium, 2011) 2. Flammability limits of CH 4 /air mixtures at elevated pressures» (33 rd Combustion Symposium, 2011) 3. Propagation of flames of butanol isomers» (33 rd Combustion Symposium, 2011) 4. Extinction of DME and ethanol flames» (33 rd Combustion Symposium, 2011) 5. Propagation and extinction of flames of methanol, ethanol, and n-butanol» (Combustion and Flame, 2011) 6. Propagation of flames of n-propanol, iso-propanol, and propane» (Combustion and Flame, 2011) 7. Propagation and extinction of flames of C 4 and C 10 methyl-esters» (Combustion and Flame, 2011)
10 Progress During Year 2 1. Propagation of flames of C 1 -C 4 methyl and ethyl esters» (in preparation; lead investigator: Lee Wang) 2. Propagation of flames of C 3 and C 4 ketones and aldehydes» (in preparation; lead investigator: Peter Veloo) 3. Propagation of flames of C 3 and C 4 hydrocarbons» (in preparation; lead investigators: Okjoo Park & Peter Veloo) 4. Comparative soot studies in flames of C 2 -C 11 methyl and ethyl esters and corresponding n-alkanes» (in preparation; lead investigators: Qiayo Feng & Aydin Jalali) 5. Comparative NO x studies in flames of C 1 -C 11 methyl and ethyl esters and corresponding n-alkanes» (in preparation; lead investigator: Qiyao Feng)
11 C 1 -C 4 Methyl and Ethyl Ester Flames 1. Fuels: Methyl Formate: Ethyl Formate: Methyl Acetate: Ethyl Acetate: Methyl Propionate: Ethyl Propionate: Methyl Butanoate: 2. Kinetic models: C.K. Westbrook, W.J. Pitz, P.R. Westmoreland, F.L. Dryer, M. Chaos, P. Osswald, K. Kohse-Höinghaus, T.A. Cool, J. Wang, B. Yang, N. Hansen, T. Kasper, Proc. Combust. Inst. 32 (2009) B. Yang, C.K. Westbrook, T. A. Cool, N. Hansen, K. Kohse-Höinghaus, "Fuel-Specific Influences on the Composition of Reaction Intermediates in Premixed Flames of Three C 5 H 10 O 2 Ester Isomers", submitted for publication, G. Bourque, D. Healy, H.J. Curran, C. Zinner, D. Kalitan, J. de Vries, C. Aul, E. Petersen, Proc. ASME Turbo. Expo. 3 (2008) Wang and coworkers: USC Mech II kinetic model.
12 Methyl Formate/Air Flames Proprietary data and not shown here Proprietary data and not shown here
13 Methyl Acetate/Air Flames Proprietary data and not shown here
14 Methyl Propionate/Air Flames Proprietary data and not shown here
15 Methyl Butanoate/Air Flames Proprietary data and not shown here
16 Ethyl Formate/Air Flames Proprietary data and not shown here
17 Ethyl Acetate/Air Flames Proprietary data and not shown here
18 Ethyl Propionate/Air Flames Proprietary data and not shown here
19 Methyl Ester/Air Flames Proprietary data and not shown here
20 Ethyl Ester/Air Flames Proprietary data and not shown here
21 C 3 -C 4 Ketone and Aldehyde Flames 1. Fuels: 2. Kinetic models: C.K. Westbrook Wang and coworkers: USC Mech II kinetic model.
22 Acetone/Air and Butanone/Air Flames Proprietary data and not shown here Compared to butanone, acetone flame produce notably higher levels of CH 3
23 Comparison of Acetone/Air Laminar Flame Speeds Proprietary data and not shown here
24 Propanal/Air and n-butanal/air Flames Proprietary data and not shown here
25 n-butanal/air and iso-butanal/air Flames Proprietary data and not shown here
26 Propanal/Air and Acetone/Air Flames Proprietary data and not shown here
27 n-butanal/air and Butanone/Air Flames Proprietary data and not shown here Similar to the C 3 compounds, the aldehyde functional group enhances reactivity compared to the ketone group. The reactivity difference appears to be diminished as the carbon number increases.
28 Soot Studies in C 2 -C 11 Methyl and Ethyl Ester Flames 1. Fuels: Diesel Biodiesel (Law and coworkers) 2. Kinetic models: C.K. Westbrook, W.J. Pitz, P.R. Westmoreland, F.L. Dryer, M. Chaos, P. Osswald, K. Kohse-Höinghaus, T.A. Cool, J. Wang, B. Yang, N. Hansen, T. Kasper, Proc. Combust. Inst. 32 (2009) B. Yang, C.K. Westbrook, T. A. Cool, N. Hansen, K. Kohse-Höinghaus, "Fuel-Specific Influences on the Composition of Reaction Intermediates in Premixed Flames of Three C 5 H 10 O 2 Ester Isomers", submitted for publication, L.K. Huynh, A. Violi. J., Org. Chem. 73 (2008) K. Seshadri, T. Lu, O. Herbinet, S. Humer, U. Niemann, W.J. Pitz, R. Seiser, C.K. Law, Proc. Comb. Inst. 32 (2009) Wang and coworkers: USC Mech II and JetSurf 2.0 kinetic models.
29 Effect of Carbon Number on Sooting Propensity of Ester Flames Proprietary data and not shown here Proprietary data and not shown here Proprietary data and not shown here
30 Effect of Carbon Number on Sooting Propensity of n-alkane Flames Proprietary data and not shown here Proprietary data and not shown here
31 Sooting Propensity of Methyl Ester and n-alkane Flames Proprietary data and not shown here Proprietary data and not shown here Proprietary data and not shown here Proprietary data and not shown here Proprietary data and not shown here
32 Sooting Propensity of Ethyl Ester and n-alkane Flames Proprietary data and not shown here Proprietary data and not shown here
33 Sooting Propensity of Methyl and Ethyl Ester Flames Proprietary data and not shown here Proprietary data and not shown here Proprietary data and not shown here
34 Sooting Propensity of Saturated and Unsaturated Methyl Ester Flames Proprietary data and not shown here Proprietary data and not shown here Proprietary data and not shown here
35 Sooting Propensity of Diesel Surrogate and Large Ester Flames Diesel surrogate: 70% n-c 10 H % 1-methyl naphthalene Dagaut and coworkers (2010) Proprietary data and not shown here Diesel Biodiesel (Law and coworkers)
36 Analysis of Computed Flame Structures 1. Comparing methyl esters and n-alkanes: Mole fractions of C 2 H 2 and C 3 H 3 consistently higher in n-alkane flames for the same reactant composition and same maximum flame temperature Early CO 2 formation in methyl esters results in less carbon that is available for soot formation 2. Comparing methyl and ethyl esters with the same carbon numbers: The higher propensity of ethyl ester flames cannot be explained consistently based on the concentrations of C 2 H 2 and C 3 H Comparing saturated and unsaturated methyl esters: Mole fractions of C 2 H 2 and C 3 H 3 consistently higher in unsaturated methyl ester flames for the same reactant composition and same maximum flame temperature
37 Concluding Remarks 1. Fundamental flame properties were investigated experimentally and computationally at atmospheric pressure for:» alcohols (C 1 -C 4 )» methyl and ethyl esters (C 1 -C 11 )» ketones (C 3 -C 4 )» aldehydes (C 3 -C 4 )» n-alkanes (C 3 -C 4 ) 2. The effects of O-containing functional group, carbon number, branching, and extent of saturation were assessed on:» flame propagation and extinction» NO x formation propensity» soot formation propensity 3. Notable deficiencies were identified in various existing models attributed to:» fuel-related kinetics» (foundation) C 0 -C 4 kinetics» fuel transport properties
38 n-butanol Proprietary data and not shown here
Ulrich Niemann a, Reinhard Seiser a & Kalyanasundaram Seshadri a a Department of Mechanical and Aerospace Engineering,
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