Multi-species time-history measurements during high-temperature acetone and 2-butanone pyrolysis

Handle URI:
http://hdl.handle.net/10754/562581
Title:
Multi-species time-history measurements during high-temperature acetone and 2-butanone pyrolysis
Authors:
Lam, Kingyiu; Ren, Wei; Pyun, Sunghyun; Farooq, Aamir ( 0000-0001-5296-2197 ) ; Davidson, David Frank; Hanson, Ronald Kenneth
Abstract:
High-temperature acetone and 2-butanone pyrolysis studies were conducted behind reflected shock waves using five species time-history measurements (ketone, CO, CH3, CH4 and C2H4). Experimental conditions covered temperatures of 1100-1600 Kat 1.6 atm, for mixtures of 0.25-1.5% ketone in argon. During acetone pyrolysis, the CO concentration time-history was found to be strongly sensitive to the acetone dissociation rate constant κ1 (CH3COCH3 → CH3 + CH3CO), and this could be directly determined from the CO time-histories, yielding κ1(1.6 atm) = 2.46 × 1014 exp(-69.3 [kcal/mol]/RT) s-1 with an uncertainty of ±25%. This rate constant is in good agreement with previous shock tube studies from Sato and Hidaka (2000) [3] and Saxena et al. (2009) [4] (within 30%) at temperatures above 1450 K, but is at least three times faster than the evaluation from Sato and Hidaka at temperatures below 1250 K. Using this revised κ1 value with the recent mechanism of Pichon et al. (2009) [5], the simulated profiles during acetone pyrolysis show excellent agreement with all five species time-history measurements. Similarly, the overall 2-butanone decomposition rate constant κtot was inferred from measured 2-butanone time-histories, yielding κ tot(1.5 atm) = 6.08 × 1013 exp(-63.1 [kcal/mol]/RT) s -1 with an uncertainty of ±35%. This rate constant is approximately 30% faster than that proposed by Serinyel et al. (2010) [11] at 1119 K, and approximately 100% faster at 1412 K. Using the measured 2-butanone and CO time-histories and an O-atom balance analysis, a missing removal pathway for methyl ketene was identified. The rate constant for the decomposition of methyl ketene was assumed to be the same as the value for the ketene decomposition reaction. Using the revised κtot value and adding the methyl ketene decomposition reaction to the Serinyel et al. mechanism, the simulated profiles during 2-butanone pyrolysis show good agreement with the measurements for all five species. © 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved.
KAUST Department:
Clean Combustion Research Center; Physical Sciences and Engineering (PSE) Division; Mechanical Engineering Program; Chemical Kinetics & Laser Sensors Laboratory
Publisher:
Elsevier
Journal:
Proceedings of the Combustion Institute
Issue Date:
Jan-2013
DOI:
10.1016/j.proci.2012.06.009
Type:
Article
ISSN:
15407489
Sponsors:
This work was supported by the US Department of Energy, Basic Energy Sciences (DE-FG02-88ER13857) with Dr. Wade Sisk as program manager.
Appears in Collections:
Articles; Physical Sciences and Engineering (PSE) Division; Mechanical Engineering Program; Clean Combustion Research Center

Full metadata record

DC FieldValue Language
dc.contributor.authorLam, Kingyiuen
dc.contributor.authorRen, Weien
dc.contributor.authorPyun, Sunghyunen
dc.contributor.authorFarooq, Aamiren
dc.contributor.authorDavidson, David Franken
dc.contributor.authorHanson, Ronald Kennethen
dc.date.accessioned2015-08-03T10:43:37Zen
dc.date.available2015-08-03T10:43:37Zen
dc.date.issued2013-01en
dc.identifier.issn15407489en
dc.identifier.doi10.1016/j.proci.2012.06.009en
dc.identifier.urihttp://hdl.handle.net/10754/562581en
dc.description.abstractHigh-temperature acetone and 2-butanone pyrolysis studies were conducted behind reflected shock waves using five species time-history measurements (ketone, CO, CH3, CH4 and C2H4). Experimental conditions covered temperatures of 1100-1600 Kat 1.6 atm, for mixtures of 0.25-1.5% ketone in argon. During acetone pyrolysis, the CO concentration time-history was found to be strongly sensitive to the acetone dissociation rate constant κ1 (CH3COCH3 → CH3 + CH3CO), and this could be directly determined from the CO time-histories, yielding κ1(1.6 atm) = 2.46 × 1014 exp(-69.3 [kcal/mol]/RT) s-1 with an uncertainty of ±25%. This rate constant is in good agreement with previous shock tube studies from Sato and Hidaka (2000) [3] and Saxena et al. (2009) [4] (within 30%) at temperatures above 1450 K, but is at least three times faster than the evaluation from Sato and Hidaka at temperatures below 1250 K. Using this revised κ1 value with the recent mechanism of Pichon et al. (2009) [5], the simulated profiles during acetone pyrolysis show excellent agreement with all five species time-history measurements. Similarly, the overall 2-butanone decomposition rate constant κtot was inferred from measured 2-butanone time-histories, yielding κ tot(1.5 atm) = 6.08 × 1013 exp(-63.1 [kcal/mol]/RT) s -1 with an uncertainty of ±35%. This rate constant is approximately 30% faster than that proposed by Serinyel et al. (2010) [11] at 1119 K, and approximately 100% faster at 1412 K. Using the measured 2-butanone and CO time-histories and an O-atom balance analysis, a missing removal pathway for methyl ketene was identified. The rate constant for the decomposition of methyl ketene was assumed to be the same as the value for the ketene decomposition reaction. Using the revised κtot value and adding the methyl ketene decomposition reaction to the Serinyel et al. mechanism, the simulated profiles during 2-butanone pyrolysis show good agreement with the measurements for all five species. © 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved.en
dc.description.sponsorshipThis work was supported by the US Department of Energy, Basic Energy Sciences (DE-FG02-88ER13857) with Dr. Wade Sisk as program manager.en
dc.publisherElsevieren
dc.subject2-Butanoneen
dc.subjectAcetoneen
dc.subjectLaser absorptionen
dc.subjectShock tubeen
dc.titleMulti-species time-history measurements during high-temperature acetone and 2-butanone pyrolysisen
dc.typeArticleen
dc.contributor.departmentClean Combustion Research Centeren
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentMechanical Engineering Programen
dc.contributor.departmentChemical Kinetics & Laser Sensors Laboratoryen
dc.identifier.journalProceedings of the Combustion Instituteen
dc.contributor.institutionDepartment of Mechanical Engineering, Stanford University, 452 Escondido Mall, Stanford, CA 94305-3032, United Statesen
kaust.authorFarooq, Aamiren
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