Startseite Naturwissenschaften Isomer Identification in Flames with Double-Imaging Photoelectron/Photoion Coincidence Spectroscopy (i2PEPICO) using Measured and Calculated Reference Photoelectron Spectra
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Isomer Identification in Flames with Double-Imaging Photoelectron/Photoion Coincidence Spectroscopy (i2PEPICO) using Measured and Calculated Reference Photoelectron Spectra

  • Julia Pieper EMAIL logo , Steffen Schmitt , Christian Hemken , Emma Davies , Julia Wullenkord , Andreas Brockhinke , Julia Krüger , Gustavo A. Garcia , Laurent Nahon , Arnas Lucassen , Wolfgang Eisfeld und Katharina Kohse-Höinghaus EMAIL logo
Veröffentlicht/Copyright: 23. Oktober 2017
Zeitschrift für Physikalische Chemie
Aus der Zeitschrift Zeitschrift für Physikalische Chemie Band 232 Heft 2

Abstract

Double-imaging photoelectron/photoion coincidence (i2PEPICO) spectroscopy using a multiplexing, time-efficient, fixed-photon-energy approach offers important opportunities of gas-phase analysis. Building on successful applications in combustion systems that have demonstrated the discriminative power of this technique, we attempt here to push the limits of its application further to more chemically complex combustion examples. The present investigation is devoted to identifying and potentially quantifying compounds featuring five heavy atoms in laminar, premixed low-pressure flames of hydrocarbon and oxygenated fuels and their mixtures. In these combustion examples from flames of cyclopentene, iso-pentane, iso-pentane blended with dimethyl ether (DME), and diethyl ether (DEE), we focus on the unambiguous assignment and quantitative detection of species with the sum formulae C5H6, C5H7, C5H8, C5H10, and C4H8O in the respective isomer mixtures, attempting to provide answers to specific chemical questions for each of these examples. To analyze the obtained i2PEPICO results from these combustion situations, photoelectron spectra (PES) from pure reference compounds, including several examples previously unavailable in the literature, were recorded with the same experimental setup as used in the flame measurements. In addition, PES of two species where reference spectra have not been obtained, namely 2-methyl-1-butene (C5H10) and the 2-cyclopentenyl radical (C5H7), were calculated on the basis of high-level ab initio calculations and Franck-Condon (FC) simulations. These reference measurements and quantum chemical calculations support the early fuel decomposition scheme in the cyclopentene flame towards 2-cyclopentenyl as the dominant fuel radical as well as the prevalence of branched intermediates in the early fuel destruction reactions in the iso-pentane flame, with only minor influences from DME addition. Furthermore, the presence of ethyl vinyl ether (EVE) in DEE flames that was predicted by a recent DEE combustion mechanism could be confirmed unambiguously. While combustion measurements using i2PEPICO can be readily obtained in isomer-rich situations, we wish to highlight the crucial need for high-quality reference information to assign and evaluate the obtained spectra.

Keywords: 3-buten-1-ol; 3-buten-2-ol; combustion chemistry; cyclopentadiene; cyclopentene; 2-cyclopentenyl radical; ethyl vinyl ether; iso-butanal; iso-butenol; laminar flames; 2-methoxypropene; 2-methyl-1-buten-3-yne; 2-methyl-1-butene; 2-methyl-2-butene; 3-methyl-1-butene; methyl ethyl ketone; n-butanal; 1,3-pentadiene; 1,4-pentadiene; 1-pentene; 2-pentene; PEPICO; photoelectron spectra; tetrahydrofuran
Corresponding authors: Julia Pieper and Katharina Kohse-Höinghaus, Physical Chemistry I, Bielefeld University, Universitätsstraße 25, 33615 Bielefeld, Germany, Phone: +49 521 106 6308 (J. Pieper); +49 521 106 2052 (K. Kohse-Höinghaus), Fax: +49 521 106 15 6887

Acknowledgments

The experiments at the SOLEIL synchrotron were performed under proposal 20150205. We would like to thank the SOLEIL staff for smoothly running the facility and for ongoing support during our measurements. In particular, we appreciate the technical help provided by Jean-François Gil. We wish to thank Dr. Michael Letzgus for programming support with the numerical minimization procedure.

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Supplemental Material:

The online version of this article offers supplementary material (https://doi.org/10.1515/zpch-2017-1009).

Received: 2017-7-11
Accepted: 2017-8-31
Published Online: 2017-10-23
Published in Print: 2018-2-23

©2018 Walter de Gruyter GmbH, Berlin/Boston

Artikel in diesem Heft

  1. Frontmatter
  2. Isomer Identification in Flames with Double-Imaging Photoelectron/Photoion Coincidence Spectroscopy (i2PEPICO) using Measured and Calculated Reference Photoelectron Spectra
  3. Electrochemical Lignin Degradation in Ionic Liquids on Ternary Mixed Metal Electrodes
  4. Novel Design, Preparation, Characterization and Antimicrobial Activity of Silver Nanoparticles during Oak Acorns Bark Retrograde
  5. Mn(II) Catalyzed Oxidation of Atenolol by Cerium(IV) in Aqueous Sulfuric Acid Medium: A Spectrophotometer Aided Kinetic, Mechanistic and Thermodynamic Study
  6. Synthesis of Nanostructured Tin Oxide by Sol–Gel and Sonochemical Approaches in an Ionic Liquid
  7. Solubility and Preferential Solvation of Piroxicam in Neat Solvents and Binary Systems
  8. Study on Host-Guest Inclusion Complexation of a Drug in Cucurbit [6]uril
  9. Discovery of a Unique Sinusoidal Frequency for the Effective Magnetic Treatment of Brackish Water
https://doi.org/10.1515/zpch-2017-1009
Schlagwörter für diesen Artikel
3-buten-1-ol; 3-buten-2-ol; combustion chemistry; cyclopentadiene; cyclopentene; 2-cyclopentenyl radical; ethyl vinyl ether; iso-butanal; iso-butenol; laminar flames; 2-methoxypropene; 2-methyl-1-buten-3-yne; 2-methyl-1-butene; 2-methyl-2-butene; 3-methyl-1-butene; methyl ethyl ketone; n-butanal; 1,3-pentadiene; 1,4-pentadiene; 1-pentene; 2-pentene; PEPICO; photoelectron spectra; tetrahydrofuran

Artikel in diesem Heft

  1. Frontmatter
  2. Isomer Identification in Flames with Double-Imaging Photoelectron/Photoion Coincidence Spectroscopy (i2PEPICO) using Measured and Calculated Reference Photoelectron Spectra
  3. Electrochemical Lignin Degradation in Ionic Liquids on Ternary Mixed Metal Electrodes
  4. Novel Design, Preparation, Characterization and Antimicrobial Activity of Silver Nanoparticles during Oak Acorns Bark Retrograde
  5. Mn(II) Catalyzed Oxidation of Atenolol by Cerium(IV) in Aqueous Sulfuric Acid Medium: A Spectrophotometer Aided Kinetic, Mechanistic and Thermodynamic Study
  6. Synthesis of Nanostructured Tin Oxide by Sol–Gel and Sonochemical Approaches in an Ionic Liquid
  7. Solubility and Preferential Solvation of Piroxicam in Neat Solvents and Binary Systems
  8. Study on Host-Guest Inclusion Complexation of a Drug in Cucurbit [6]uril
  9. Discovery of a Unique Sinusoidal Frequency for the Effective Magnetic Treatment of Brackish Water
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Heruntergeladen am 15.3.2026 von https://www.degruyterbrill.com/document/doi/10.1515/zpch-2017-1009/html
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