Benzene formation in premixed fuel-rich 1,3-butadiene flames

Hansen, Nils; Miller, James A.; Kasper, Tina; Kohse-Höinghaus, Katharina; Westmoreland, Phillip R.; Wang, Juan; Cool, Terrill A.

doi:10.1016/j.proci.2008.06.050

Benzene formation in premixed fuel-rich 1,3-butadiene flames

Journal Article · Sun Sep 14 04:00:00 EDT 2008 · Proceedings of the Combustion Institute

DOI:https://doi.org/10.1016/j.proci.2008.06.050· OSTI ID:1060548

Hansen, Nils ^[1]; Miller, James A.; Kasper, Tina; Kohse-Höinghaus, Katharina; Westmoreland, Phillip R.; Wang, Juan; Cool, Terrill A.

Combustion Research Facility, Sandia National Laboratories, Livermore, CA 94551

Detailed kinetic modeling and flame-sampling molecular-beam time-of-flight mass spectrometry are combined to unravel important pathways leading to the formation of benzene in a premixed laminar low-pressure 1,3-butadiene flame. The chemical kinetic model developed is compared with new experimental results obtained for a rich (phi = 1.8) 1,3-butudiene/O(2)/Ar flame at 30 Torr and with flame data for a similar but richer (phi = 2.4) flame reported by Cole et al. [Combust. Flame 56 (1) (1984) 51-70]. The newer experiment utilizes photoionization by tunable vacuum-ultraviolet synchrotron radiation, which allows for the identification and separation of combustion species by their characteristic ionization energies. Predictions of mole fractions as a function of distance from the burner of major combustion intermediates and products are in overall satisfactory agreement with experimentally observed profiles. The accurate predictions of the propargyl radical and benzene mole fractions permit an assessment of potential benzene formation pathways. The results indicate that C(6)H(6) is formed mainly by the C(3)H(3) + C(3)H(3) and i-C(4)H(5) + C(2)H(2) reactions, which are roughly of equal importance. Smaller contributions arise from C(3)H(3) + C(3)H(5). However, given the experimental and modeling uncertainties, other pathways cannot be ruled out.

Research Organization:: Cornell Univ., Ithaca, NY (United States)

Sponsoring Organization:: USDOE IG Office of Audit Services (IG-30)

DOE Contract Number:: FG02-01ER15180

OSTI ID:: 1060548

Report Number(s):: DOE-ER15180-15

Journal Information:: Proceedings of the Combustion Institute, Journal Name: Proceedings of the Combustion Institute Journal Issue: 1 Vol. 32; ISSN 1540-7489

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

References (36)

Noncatalytic thermocouple coatings produced with chemical vapor deposition for flame temperature measurements Bahlawane, N.; Struckmeier, U.; Kasper, T. S. Review of Scientific Instruments, Vol. 78, Issue 1 https://doi.org/10.1063/1.2426876	journal	January 2007
Initial Steps of Aromatic Ring Formation in a Laminar Premixed Fuel-Rich Cyclopentene Flame† Hansen, N.; Kasper, T.; Klippenstein, S. J. The Journal of Physical Chemistry A, Vol. 111, Issue 19 https://doi.org/10.1021/jp0683317	journal	May 2007
On the Combination Reactions of Hydrogen Atoms with Resonance-Stabilized Hydrocarbon Radicals ^† Harding, Lawrence B.; Klippenstein, Stephen J.; Georgievskii, Yuri The Journal of Physical Chemistry A, Vol. 111, Issue 19 https://doi.org/10.1021/jp0682309	journal	May 2007
Formation mechanisms of aromatic compounds in aliphatic flames Cole, J. A.; Bittner, J. D.; Longwell, J. P. Combustion and Flame, Vol. 56, Issue 1 https://doi.org/10.1016/0010-2180(84)90005-1	journal	April 1984
Oxidation pathways in the reaction of diacetylene with OH radicals Senosiain, Juan P.; Klippenstein, Stephen J.; Miller, James A. Proceedings of the Combustion Institute, Vol. 31, Issue 1 https://doi.org/10.1016/j.proci.2006.08.084	journal	January 2007
Kinetic modeling of counterflow diffusion flames of butadiene Granata, Silvia; Faravelli, Tiziano; Ranzi, Eliseo Combustion and Flame, Vol. 131, Issue 3 https://doi.org/10.1016/S0010-2180(02)00407-8	journal	November 2002
Unravelling combustion mechanisms through a quantitative understanding of elementary reactions Miller, James A.; Pilling, Michael J.; Troe, Jürgen Proceedings of the Combustion Institute, Vol. 30, Issue 1 https://doi.org/10.1016/j.proci.2004.08.281	journal	January 2005
Master Equation Methods in Gas Phase Chemical Kinetics Miller, James A.; Klippenstein, Stephen J. The Journal of Physical Chemistry A, Vol. 110, Issue 36 https://doi.org/10.1021/jp062693x	journal	September 2006
Effect of oxygen addition on polycyclic aromatic hydrocarbon formation in 1,3 butadiene counter-Flow diffusion flames Olten, Nesrin; Senkan, Selim Combustion and Flame, Vol. 125, Issue 1-2 https://doi.org/10.1016/S0010-2180(01)00224-3	journal	April 2001
Rich premixed laminar methane flames doped by light unsaturated hydrocarbons Gueniche, H. A.; Glaude, P. A.; Fournet, R. Combustion and Flame, Vol. 151, Issue 1-2 https://doi.org/10.1016/j.combustflame.2007.05.007	journal	October 2007
An ab Initio/RRKM Study of Product Branching Ratios in the Photodissociation of Buta-1,2- and -1,3-dienes and But-2-yne at 193 nm Lee, Hwa-Yu; Kislov, Vadim V.; Lin, Sheng-Hsien Chemistry - A European Journal, Vol. 9, Issue 3 https://doi.org/10.1002/chem.200390081	journal	February 2003
Molecular beam mass spectrometry for studying the fundamental chemistry of flames Biordi, Joan C. Progress in Energy and Combustion Science, Vol. 3, Issue 3 https://doi.org/10.1016/0360-1285(77)90002-8	journal	January 1977
Species and Soot Concentration Measurements in a Methane/Air Nonpremixed Flame Doped With C4 Hydrocarbons McEnally, Charles S.; Pfefferle, Lisa D. Combustion and Flame, Vol. 115, Issue 1-2 https://doi.org/10.1016/S0010-2180(97)00348-9	journal	October 1998
Combustion Chemistry of Enols: Possible Ethenol Precursors in Flames ^† Taatjes, Craig A.; Hansen, Nils; Miller, James A. The Journal of Physical Chemistry A, Vol. 110, Issue 9 https://doi.org/10.1021/jp0547313	journal	March 2006
The Reaction of n - and i -C ₄ H ₅ Radicals with Acetylene ^† Senosiain, Juan P.; Miller, James A. The Journal of Physical Chemistry A, Vol. 111, Issue 19 https://doi.org/10.1021/jp0675126	journal	May 2007
The Oxidation of 1,3-Butadiene: Experimental Results and Kinetic Modeling Dagaut*, P.; Cathonnet, M. Combustion Science and Technology, Vol. 140, Issue 1-6 https://doi.org/10.1080/00102209808915773	journal	December 1998
The Recombination of Propargyl Radicals and Other Reactions on a C ₆ H ₆ Potential Miller, James A.; Klippenstein, Stephen J. The Journal of Physical Chemistry A, Vol. 107, Issue 39 https://doi.org/10.1021/jp030375h	journal	October 2003
Photoionization mass spectrometer for studies of flame chemistry with a synchrotron light source Cool, Terrill A.; McIlroy, Andrew; Qi, Fei Review of Scientific Instruments, Vol. 76, Issue 9 https://doi.org/10.1063/1.2010307	journal	September 2005
Experimental counterflow ignition temperatures and reaction mechanisms of 1,3-butadiene Zheng, X. L.; Lu, T. F.; Law, C. K. Proceedings of the Combustion Institute, Vol. 31, Issue 1 https://doi.org/10.1016/j.proci.2006.07.182	journal	January 2007
Reactions over Multiple, Interconnected Potential Wells: Unimolecular and Bimolecular Reactions on a C ₃ H ₅ Potential ^† Miller, James A.; Senosiain, Juan P.; Klippenstein, Stephen J. The Journal of Physical Chemistry A, Vol. 112, Issue 39 https://doi.org/10.1021/jp804510k	journal	October 2008
A study of benzene formation in a laminar flow reactor Skjøth-Rasmussen, M. S.; Glarborg, P.; Østberg, M. Proceedings of the Combustion Institute, Vol. 29, Issue 1 https://doi.org/10.1016/S1540-7489(02)80163-8	journal	January 2002
Isomer-Specific Fuel Destruction Pathways in Rich Flames of Methyl Acetate and Ethyl Formate and Consequences for the Combustion Chemistry of Esters ^† Osswald, Patrick; Struckmeier, Ulf; Kasper, Tina The Journal of Physical Chemistry A, Vol. 111, Issue 19 https://doi.org/10.1021/jp068337w	journal	May 2007
Experimental and modeling of oxidation of acetylene, propyne, allene and 1,3-butadiene Fournet, R.; Bauge, J. C.; Battin-Leclerc, F. International Journal of Chemical Kinetics, Vol. 31, Issue 5 https://doi.org/10.1002/(SICI)1097-4601(1999)31:5<361::AID-KIN6>3.0.CO;2-K	journal	January 1999
Studies of a fuel-rich propane flame with photoionization mass spectrometry Cool, Terrill A.; Nakajima, Koichi; Taatjes, Craig A. Proceedings of the Combustion Institute, Vol. 30, Issue 1 https://doi.org/10.1016/j.proci.2004.08.103	journal	January 2005
Benzene precursors and formation routes in a stoichiometric cyclohexane flame Law, Matthew E.; Westmoreland, Phillip R.; Cool, Terrill A. Proceedings of the Combustion Institute, Vol. 31, Issue 1 https://doi.org/10.1016/j.proci.2006.07.259	journal	January 2007
Kinetic and thermodynamic issues in the formation of aromatic compounds in flames of aliphatic fuels Miller, James A.; Melius, Carl F. Combustion and Flame, Vol. 91, Issue 1 https://doi.org/10.1016/0010-2180(92)90124-8	journal	October 1992
The effects of premixing on soot production in nonpremixed flames fueled with unsaturated hydrocarbons McEnally, Charles S.; Pfefferle, Lisa D. Proceedings of the Combustion Institute, Vol. 29, Issue 2 https://doi.org/10.1016/S1540-7489(02)80293-0	journal	January 2002
Laser Studies of Small Radicals in Rich Methane Flames: OH, HCO, and ¹ CH ₂ McIlroy, Andrew Israel Journal of Chemistry, Vol. 39, Issue 1 https://doi.org/10.1002/ijch.199900006	journal	January 1999
Studies of aromatic hydrocarbon formation mechanisms in flames: Progress towards closing the fuel gap McEnally, Charles S.; Pfefferle, Lisa D.; Atakan, Burak Progress in Energy and Combustion Science, Vol. 32, Issue 3 https://doi.org/10.1016/j.pecs.2005.11.003	journal	January 2006
A Comparative Study of the Kinetics of Benzene Formation from Unsaturated C2 to C4 Hydrocarbons Dagaut, P. Combustion and Flame, Vol. 113, Issue 4 https://doi.org/10.1016/S0010-2180(97)00244-7	journal	June 1998
Association rate constants for reactions between resonance-stabilized radicals: C3H3 + C3H3, C3H3 + C3H5, and C3H5 + C3H5 Georgievskii, Yuri; Miller, James A.; Klippenstein, Stephen J. Physical Chemistry Chemical Physics, Vol. 9, Issue 31 https://doi.org/10.1039/b703261g	journal	January 2007
Identification and Chemistry of C ₄ H ₃ and C ₄ H ₅ Isomers in Fuel-Rich Flames Hansen, Nils; Klippenstein, Stephen J.; Taatjes, Craig A. The Journal of Physical Chemistry A, Vol. 110, Issue 10 https://doi.org/10.1021/jp056769l	journal	March 2006
Detailed kinetic modeling of 1,3-butadiene oxidation at high temperatures Laskin, Alexander; Wang, Hai; Law, Chung K. International Journal of Chemical Kinetics, Vol. 32, Issue 10 https://doi.org/10.1002/1097-4601(2000)32:10<589::AID-KIN2>3.0.CO;2-U	journal	January 2000
Photoionization mass spectrometric studies and modeling of fuel-rich allene and propyne flames Hansen, Nils; Miller, James A.; Taatjes, Craig A. Proceedings of the Combustion Institute, Vol. 31, Issue 1 https://doi.org/10.1016/j.proci.2006.07.045	journal	January 2007
Benene formation chemistry in premixed 1,3-butadiene flames Lindstedt, R. P.; Skevis, G. Symposium (International) on Combustion, Vol. 26, Issue 1 https://doi.org/10.1016/S0082-0784(96)80278-5	journal	January 1996
The high temperature oxidation of butadiene Brezinsky, K.; Burke, E. J.; Glassman, I. Symposium (International) on Combustion, Vol. 20, Issue 1 https://doi.org/10.1016/S0082-0784(85)80550-6	journal	January 1985

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3-Butadiene
10 SYNTHETIC FUELS
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ACETYLENE
AROMATIC-HYDROCARBON FORMATION
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Benzene formation in premixed fuel-rich 1,3-butadiene flames

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