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

Julia Pieper; Steffen Schmitt; Christian Hemken; Emma Davies; Julia Wullenkord; Andreas Brockhinke; Julia Krüger; Gustavo A. Garcia; Laurent Nahon; Arnas Lucassen; Wolfgang Eisfeld; Katharina Kohse-Höinghaus

doi:10.1515/zpch-2017-1009

Published by De Gruyter (O) October 23, 2017

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

Julia Pieper , Steffen Schmitt , Christian Hemken , Emma Davies , Julia Wullenkord , Andreas Brockhinke , Julia Krüger , Gustavo A. Garcia , Laurent Nahon , Arnas Lucassen , Wolfgang Eisfeld and Katharina Kohse-Höinghaus

From the journal Zeitschrift für Physikalische Chemie

https://doi.org/10.1515/zpch-2017-1009

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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.

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