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Title: Influences of the molecular fuel structure on combustion reactions towards soot precursors in selected alkane and alkene flames

Abstract

In this paper, we experimentally investigate the high-temperature oxidation kinetics of n-pentane, 1-pentene and 2-methyl-2-butene (2M2B) in a combustion environment using flame-sampling molecular beam mass spectrometry. The selected C 5 fuels are prototypes for linear and branched, saturated and unsaturated fuel components, featuring different C–C and C–H bond structures. It is shown that the formation tendency of species, such as polycyclic aromatic hydrocarbons (PAHs), yielded through mass growth reactions increases drastically in the sequence n-pentane < 1-pentene < 2M2B. This comparative study enables valuable insights into fuel-dependent reaction sequences of the gas-phase combustion mechanism that provide explanations for the observed difference in the PAH formation tendency. First, we investigate the fuel-structure-dependent formation of small hydrocarbon species that are yielded as intermediate species during the fuel decomposition, because these species are at the origin of the subsequent mass growth reaction pathways. Second, we review typical PAH formation reactions inspecting repetitive growth sequences in dependence of the molecular fuel structure. Third, we discuss how differences in the intermediate species pool influence the formation reactions of key aromatic ring species that are important for the PAH growth process underlying soot formation. Finally, as a main result it was found that for the fuelsmore » featuring a C=C double bond, the chemistry of their allylic fuel radicals and their decomposition products strongly influences the combination reactions to the initially formed aromatic ring species and as a consequence, the PAH formation tendency.« less

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3];  [1]
  1. Bielefeld Univ. (Germany). Dept. of Chemistry
  2. Physikalisch-Technische Bundesanstalt (PTB), Braunschweig (Germany); Sandia National Lab. (SNL-CA), Livermore, CA (United States). Combustion Research Facility
  3. Sandia National Lab. (SNL-CA), Livermore, CA (United States). Combustion Research Facility
Publication Date:
Research Org.:
Sandia National Lab. (SNL-CA), Livermore, CA (United States); Bielefeld Univ. (Germany)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA); German Research Foundation (DFG)
OSTI Identifier:
1474088
Report Number(s):
SAND-2018-10260J
Journal ID: ISSN 1463-9076; 667994
Grant/Contract Number:  
NA0003525; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 20; Journal Issue: 16; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Ruwe, Lena, Moshammer, Kai, Hansen, Nils, and Kohse-Höinghaus, Katharina. Influences of the molecular fuel structure on combustion reactions towards soot precursors in selected alkane and alkene flames. United States: N. p., 2018. Web. doi:10.1039/C7CP07743B.
Ruwe, Lena, Moshammer, Kai, Hansen, Nils, & Kohse-Höinghaus, Katharina. Influences of the molecular fuel structure on combustion reactions towards soot precursors in selected alkane and alkene flames. United States. doi:10.1039/C7CP07743B.
Ruwe, Lena, Moshammer, Kai, Hansen, Nils, and Kohse-Höinghaus, Katharina. Fri . "Influences of the molecular fuel structure on combustion reactions towards soot precursors in selected alkane and alkene flames". United States. doi:10.1039/C7CP07743B. https://www.osti.gov/servlets/purl/1474088.
@article{osti_1474088,
title = {Influences of the molecular fuel structure on combustion reactions towards soot precursors in selected alkane and alkene flames},
author = {Ruwe, Lena and Moshammer, Kai and Hansen, Nils and Kohse-Höinghaus, Katharina},
abstractNote = {In this paper, we experimentally investigate the high-temperature oxidation kinetics of n-pentane, 1-pentene and 2-methyl-2-butene (2M2B) in a combustion environment using flame-sampling molecular beam mass spectrometry. The selected C5 fuels are prototypes for linear and branched, saturated and unsaturated fuel components, featuring different C–C and C–H bond structures. It is shown that the formation tendency of species, such as polycyclic aromatic hydrocarbons (PAHs), yielded through mass growth reactions increases drastically in the sequence n-pentane < 1-pentene < 2M2B. This comparative study enables valuable insights into fuel-dependent reaction sequences of the gas-phase combustion mechanism that provide explanations for the observed difference in the PAH formation tendency. First, we investigate the fuel-structure-dependent formation of small hydrocarbon species that are yielded as intermediate species during the fuel decomposition, because these species are at the origin of the subsequent mass growth reaction pathways. Second, we review typical PAH formation reactions inspecting repetitive growth sequences in dependence of the molecular fuel structure. Third, we discuss how differences in the intermediate species pool influence the formation reactions of key aromatic ring species that are important for the PAH growth process underlying soot formation. Finally, as a main result it was found that for the fuels featuring a C=C double bond, the chemistry of their allylic fuel radicals and their decomposition products strongly influences the combination reactions to the initially formed aromatic ring species and as a consequence, the PAH formation tendency.},
doi = {10.1039/C7CP07743B},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 16,
volume = 20,
place = {United States},
year = {2018},
month = {2}
}

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