Chemical insights into the larger sooting tendency of 2-methyl-2-butene compared to n-pentane

León, Larisa; Ruwe, Lena; Moshammer, Kai; Seidel, Lars; Shrestha, Krishna P.; Wang, Xiaoxiao; Mauss, Fabian; Kohse-Höinghaus, Katharina; Hansen, Nils

doi:10.1016/j.combustflame.2019.06.029

Title: Chemical insights into the larger sooting tendency of 2-methyl-2-butene compared to n-pentane

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Abstract

A comprehensive, chemically detailed mechanism for the combustion of 2-methyl-2-butene and n-pentane is presented to provide insights into the different sooting tendencies of these two structurally different C5 hydrocarbons. A hierarchically assembled mechanism has been developed to specifically target speciation data from low-pressure premixed flames of 2-methyl-2-butene and newly measured mole fraction data for a fuel-rich (Φ = 1.8) n-pentane flame, in which species profiles up to phenol were quantified. The partially isomer-resolved chemical composition of this flame was determined using flame-sampling molecular-beam mass spectrometry with single-photon ionization by tunable, synchrotron-generated vacuum-ultraviolet radiation. The presented model, which includes a newly determined, consistent set of the thermochemistry data for the C5 species, presents overall satisfactory capabilities to predict the mole fraction profiles of common combustion intermediates. The analysis of the model predictions revealed the fuel-structure dependencies (i.e. saturated vs. unsaturated and linear vs. branched) of the formation of small aromatic species that are considered as soot precursors. Here, the propensity of the 2-methyl-2-butene flame to form larger concentrations of aromatic species was traced back to the readily available formation routes of several small precursor molecules and the efficient formation of “first aromatic rings” beyond benzene.

Authors:

León, Larisa ^[1]; Ruwe, Lena ^[2]; Moshammer, Kai ^[3]; Seidel, Lars ^[4]; Shrestha, Krishna P. ^[1]; Wang, Xiaoxiao ^[1]; Mauss, Fabian ^[1]; Kohse-Höinghaus, Katharina ^[2]; Hansen, Nils ^[5]

Brandenburg Univ. of Technology, Cottbus (Germany)
Bielefeld Univ., Bielefeld (Germany)
Physikalisch Technische Bundesanstalt (PTB), Braunschweig (Germany)
LOGE Deutschland GmbH, Cottbus (Germany)
Sandia National Lab. (SNL-CA), Livermore, CA (United States)

Publication Date:: Thu Jul 11 00:00:00 EDT 2019

Research Org.:: Sandia National Lab. (SNL-CA), Livermore, CA (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:: 1559481

Alternate Identifier(s):: OSTI ID: 1562981

Report Number(s):: SAND-2019-5117J
Journal ID: ISSN 0010-2180; 675317

Grant/Contract Number:: AC04-94AL85000

Resource Type:: Accepted Manuscript

Journal Name:: Combustion and Flame

Additional Journal Information:: Journal Volume: 208; Journal Issue: C; Journal ID: ISSN 0010-2180

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 2-Methyl-2-butene; n-Pentane; Laminar premixed flames; Molecular-beam mass spectrometry; Kinetic modeling; PAH formation

Citation Formats


                    León, Larisa, Ruwe, Lena, Moshammer, Kai, Seidel, Lars, Shrestha, Krishna P., Wang, Xiaoxiao, Mauss, Fabian, Kohse-Höinghaus, Katharina, and Hansen, Nils. Chemical insights into the larger sooting tendency of 2-methyl-2-butene compared to n-pentane.  United States: N. p., 2019. 
Web.  doi:10.1016/j.combustflame.2019.06.029.

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                    León, Larisa, Ruwe, Lena, Moshammer, Kai, Seidel, Lars, Shrestha, Krishna P., Wang, Xiaoxiao, Mauss, Fabian, Kohse-Höinghaus, Katharina, & Hansen, Nils. Chemical insights into the larger sooting tendency of 2-methyl-2-butene compared to n-pentane.  United States.  https://doi.org/10.1016/j.combustflame.2019.06.029

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                    León, Larisa, Ruwe, Lena, Moshammer, Kai, Seidel, Lars, Shrestha, Krishna P., Wang, Xiaoxiao, Mauss, Fabian, Kohse-Höinghaus, Katharina, and Hansen, Nils. Thu .  
"Chemical insights into the larger sooting tendency of 2-methyl-2-butene compared to n-pentane".  United States.  https://doi.org/10.1016/j.combustflame.2019.06.029.  https://www.osti.gov/servlets/purl/1559481.

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@article{osti_1559481,

  title        = {Chemical insights into the larger sooting tendency of 2-methyl-2-butene compared to n-pentane},

  author       = {León, Larisa and Ruwe, Lena and Moshammer, Kai and Seidel, Lars and Shrestha, Krishna P. and Wang, Xiaoxiao and Mauss, Fabian and Kohse-Höinghaus, Katharina and Hansen, Nils},

  abstractNote = {A comprehensive, chemically detailed mechanism for the combustion of 2-methyl-2-butene and n-pentane is presented to provide insights into the different sooting tendencies of these two structurally different C5 hydrocarbons. A hierarchically assembled mechanism has been developed to specifically target speciation data from low-pressure premixed flames of 2-methyl-2-butene and newly measured mole fraction data for a fuel-rich (Φ = 1.8) n-pentane flame, in which species profiles up to phenol were quantified. The partially isomer-resolved chemical composition of this flame was determined using flame-sampling molecular-beam mass spectrometry with single-photon ionization by tunable, synchrotron-generated vacuum-ultraviolet radiation. The presented model, which includes a newly determined, consistent set of the thermochemistry data for the C5 species, presents overall satisfactory capabilities to predict the mole fraction profiles of common combustion intermediates. The analysis of the model predictions revealed the fuel-structure dependencies (i.e. saturated vs. unsaturated and linear vs. branched) of the formation of small aromatic species that are considered as soot precursors. Here, the propensity of the 2-methyl-2-butene flame to form larger concentrations of aromatic species was traced back to the readily available formation routes of several small precursor molecules and the efficient formation of “first aromatic rings” beyond benzene.},

  doi          = {10.1016/j.combustflame.2019.06.029},

  journal      = {Combustion and Flame},

  number       = C,

  volume       = 208,

  place        = {United States},

  year         = {Thu Jul 11 00:00:00 EDT 2019},

  month        = {Thu Jul 11 00:00:00 EDT 2019}

}

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