An experimental and theoretical study of pyrrolidine pyrolysis at low pressure

Arnas Lucassen, Zhandong Wang, Lidong Zhang, Feng Zhang, Wenhao Yuan, Yizun Wang, Fei Qi*, Katharina Kohse-Höinghaus

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

7 Scopus citations

Abstract

Pyrrolidine serves as a model substance for a series of saturated nitrogenated heterocycles in plants, including certain amino acids such as proline and hydroxyproline. Thus the pyrolysis of this compound was investigated regarding the increasing interest on biofuels. The pyrolysis of pyrrolidine diluted with 95% argon was studied in a flow reactor at 40 mbar over the temperature range from 950 to 1450 K. Isomer-specific assignment and quantification was performed using molecular-beam mass spectrometry and ionization with tunable synchrotron vacuum ultraviolet radiation. The prominent decomposition pathways were analyzed based on the quantified mole fractions of pyrolysis species. Computations including an ab initio calculation and kinetic modeling for the primary fuel decomposition were used to refine the analysis and reveal the combustion chemistry of this saturated heterocyclic compound. Based on the theoretical calculation, a new pathway for the isomerization reaction pyrrolidine → CH2=CHCH2CH2NH2 via a diradical intermediate was proposed. The rate constant calculations showed that this channel has a large contribution to pyrrolidine pyrolysis.

Original languageEnglish (US)
Pages (from-to)641-648
Number of pages8
JournalProceedings of the Combustion Institute
Volume34
Issue number1
DOIs
StatePublished - Jan 1 2013

Keywords

  • Biomass-related nitrogen
  • Nitrogenated fuels
  • Pyrolysis
  • Pyrrolidine
  • VUV photoionization mass spectrometry

ASJC Scopus subject areas

  • Chemical Engineering(all)
  • Mechanical Engineering
  • Physical and Theoretical Chemistry

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