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dc.contributor.authorLiu, Peng
dc.contributor.authorChen, Bingjie
dc.contributor.authorLi, Zepeng
dc.contributor.authorBennett, Anthony
dc.contributor.authorSioud, Salim
dc.contributor.authorPitsch, Heinz
dc.contributor.authorSarathy, Mani
dc.contributor.authorRoberts, William L.
dc.date.accessioned2020-09-28T08:38:10Z
dc.date.available2020-09-28T08:38:10Z
dc.date.issued2020-09-22
dc.date.submitted2019-11-04
dc.identifier.citationLiu, P., Chen, B., Li, Z., Bennett, A., Sioud, S., Pitsch, H., … Roberts, W. L. (2020). Experimental and theoretical evidence for the temperature-determined evolution of PAH functional groups. Proceedings of the Combustion Institute. doi:10.1016/j.proci.2020.07.119
dc.identifier.issn1540-7489
dc.identifier.doi10.1016/j.proci.2020.07.119
dc.identifier.urihttp://hdl.handle.net/10754/665338
dc.description.abstractElucidating the chemical evolution of various functional groups in polycyclic aromatic hydrocarbons (PAH) and soot aids in understanding soot formation chemistry. In this work, the chemical evolution of various functional groups, including aromatic Csingle bondH, aliphatic Csingle bondH, C=O, Csingle bondOH and Csingle bondOsingle bondC bonds, was experimentally investigated online, rather than with offline diagnostics. Oxidation was performed in a jet-stirred reactor (JSR), fueled with benzene/C2H2/air/N2 and benzene/phenol/C2H2/N2 for a temperature range of 600-1400 K. Kinetic modelling, including ab initio quantum chemistry calculations, reaction rate coefficient calculations and JSR simulations, were conducted to interpret the experimental data and the evolutionary chemistry of the various functional groups. Results show that the formation of functional groups on PAH and oxygenated PAH (OPAH) are highly sensitive to temperature. Aliphatic Csingle bondH bonds survive mainly in the form of Csingle bondCH2single bondC, Csingle bondCH2single bondCH2single bondC or Ctriple bondCH functional groups above 1200 K, and exist in the CHdouble bondCH2 functional group below 1000 K. For the OPAH, the Csingle bondOsingle bondC functional group presents stronger thermal stability than Csingle bondOH and C=O functional groups. Simulation results indicate that HACA-like pathway (hydrogen abstraction carbon addition), in which C2H2 attacks the O atom, followed by cyclization and H-atom elimination reactions, qualitatively describe the formation of OPAH with the Csingle bondO-C functional group at different temperatures. The addition reaction involving PAH radical and C2H4 / C2H3 captures the evolution of PAH with the CHdouble bondCH2 functional group, but fails to explain the formation of Csingle bondCH2single bondC and Csingle bondCH2single bondCH2single bondC functional groups.
dc.description.sponsorshipThe work at King Abdullah University of Science and Technology (KAUST) was supported by the KAUST Clean Fuels Consortium (KCFC) and its member companies. Calculations were run with the support of KAUST Supercomputing Lab (Shaheen & Ibex). BC and HP gratefully acknowledge financial support by the Deutsch Forschungsgemeinschaft within the framework of the collaborative research center SFB/Transregio 129 “Oxyflame”.
dc.publisherElsevier BV
dc.relation.urlhttps://linkinghub.elsevier.com/retrieve/pii/S1540748920305708
dc.rightsNOTICE: this is the author’s version of a work that was accepted for publication in Proceedings of the Combustion Institute. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Proceedings of the Combustion Institute, [, , (2020-09-22)] DOI: 10.1016/j.proci.2020.07.119 . © 2020. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0/
dc.titleExperimental and theoretical evidence for the temperature-determined evolution of PAH functional groups
dc.typeArticle
dc.contributor.departmentChemical Engineering
dc.contributor.departmentChemical Engineering Program
dc.contributor.departmentClean Combustion Research Center
dc.contributor.departmentCombustion and Pyrolysis Chemistry (CPC) Group
dc.contributor.departmentMechanical Engineering Program
dc.contributor.departmentOrganics
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.contributor.departmenthigh-pressure combustion (HPC) Research Group
dc.identifier.journalProceedings of the Combustion Institute
dc.rights.embargodate2022-09-22
dc.eprint.versionPost-print
dc.contributor.institutionInstitute for Combustion Technology, RWTH Aachen University, Templergraben 64, Aachen 52062, Germany.
kaust.personLiu, Peng
kaust.personChen, Bingjie
kaust.personLi, Zepeng
kaust.personBennett, Anthony
kaust.personSioud, Salim
kaust.personSarathy, Mani
kaust.personRoberts, William L.
dc.date.accepted2020-07-24
refterms.dateFOA2020-09-30T05:40:46Z
kaust.acknowledged.supportUnitIbex
kaust.acknowledged.supportUnitKAUST Supercomputing Lab
kaust.acknowledged.supportUnitShaheen
dc.date.published-online2020-09-22
dc.date.published-print2020-09


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