Isomer-sensitive characterization of low ...
Type de document :
Article dans une revue scientifique: Article original
DOI :
URL permanente :
Titre :
Isomer-sensitive characterization of low temperature oxidation reaction products by coupling a jet-stirred reactor to an electron/ion coincidence spectrometer: case of n-pentane
Auteur(s) :
Bourgalais, Jérémy [Auteur]
Gouid, Zied [Auteur]
Herbinet, Olivier [Auteur]
Garcia, Gustavo A. [Auteur]
Arnoux, Philippe [Auteur]
Wang, Zhandong [Auteur]
Tran, Luc-Sy [Auteur]
Physicochimie des Processus de Combustion et de l’Atmosphère - UMR 8522 [PC2A]
Vanhove, Guillaume [Auteur]
Physicochimie des Processus de Combustion et de l’Atmosphère - UMR 8522 [PC2A]
Physicochimie des Processus de Combustion et de l'Atmosphère (PC2A) - UMR 8522
Hochlaf, Majdi [Auteur]
Nahon, Laurent [Auteur]
Battin-Leclerc, Frédérique [Auteur]
Gouid, Zied [Auteur]
Herbinet, Olivier [Auteur]
Garcia, Gustavo A. [Auteur]
Arnoux, Philippe [Auteur]
Wang, Zhandong [Auteur]
Tran, Luc-Sy [Auteur]
Physicochimie des Processus de Combustion et de l’Atmosphère - UMR 8522 [PC2A]
Vanhove, Guillaume [Auteur]
Physicochimie des Processus de Combustion et de l’Atmosphère - UMR 8522 [PC2A]
Physicochimie des Processus de Combustion et de l'Atmosphère (PC2A) - UMR 8522
Hochlaf, Majdi [Auteur]
Nahon, Laurent [Auteur]
Battin-Leclerc, Frédérique [Auteur]
Titre de la revue :
Physical Chemistry Chemical Physics
Nom court de la revue :
Phys. Chem. Chem. Phys.
Numéro :
22
Pagination :
1222-1241
Éditeur :
Royal Society of Chemistry (RSC)
Date de publication :
2020-01-21
ISSN :
1463-9076
Discipline(s) HAL :
Chimie/Chimie théorique et/ou physique
Physique [physics]/Physique [physics]
Physique [physics]/Physique [physics]/Chimie-Physique [physics.chem-ph]
Physique [physics]/Physique [physics]
Physique [physics]/Physique [physics]/Chimie-Physique [physics.chem-ph]
Résumé en anglais : [en]
Through the use of tunable vacuum ultraviolet light generated by the DESIRS VUV synchrotron beamline, a jet-stirred reactor was coupled for the first time to an advanced photoionization mass spectrometer based upon a double ...
Lire la suite >Through the use of tunable vacuum ultraviolet light generated by the DESIRS VUV synchrotron beamline, a jet-stirred reactor was coupled for the first time to an advanced photoionization mass spectrometer based upon a double imaging PhotoElectron PhotoIon COincidence (i2PEPICO) scheme. This new coupling was used to investigate the low-temperature oxidation of n-pentane, a prototype molecule for gasoline or diesel fuels. Experiments were performed under quasi-atmospheric pressure (1.1 bar) with a residence time of 3 s for two equivalence ratios (1/3 and 0.5) with a fuel initial mole fraction of 0.01. The measured time-of-flight mass spectra are in good agreement with those previously obtained with other photoionization mass spectrometers and, like those previous ones, display several m/z peaks for which the related species assignation is ambiguous. This paper shows how the analysis of the coincident mass-tagged Threshold PhotoElectron Spectra (TPES) together with first principle computations, consisting of the determination of the adiabatic ionization energies and the spectra of some products, may assist products’ identification. The results mostly confirm those previously obtained by photoionization mass spectrometry and gas chromatography, but also allow a more accurate estimation of the 1-pentene/2-pentene mole fraction ratio. Our data also indicate a higher formation of acetone and methyl ethyl ketone than what is predicted by current models, as well as the presence of products that were not previously taken into account, such as methoxyacetylene, methyl vinyl ketone or furanone. The formation of three, four and five membered ring cyclic ethers is confirmed along with linear ketones: 2- and 3-pentanone. A significant general trend in indicating higher amounts of ketones than are indicated by gas chromatography is noted. Finally, TPES of alkenylhydroperoxides are also provided for the first time and constrains on the isomers identification are provided.Lire moins >
Lire la suite >Through the use of tunable vacuum ultraviolet light generated by the DESIRS VUV synchrotron beamline, a jet-stirred reactor was coupled for the first time to an advanced photoionization mass spectrometer based upon a double imaging PhotoElectron PhotoIon COincidence (i2PEPICO) scheme. This new coupling was used to investigate the low-temperature oxidation of n-pentane, a prototype molecule for gasoline or diesel fuels. Experiments were performed under quasi-atmospheric pressure (1.1 bar) with a residence time of 3 s for two equivalence ratios (1/3 and 0.5) with a fuel initial mole fraction of 0.01. The measured time-of-flight mass spectra are in good agreement with those previously obtained with other photoionization mass spectrometers and, like those previous ones, display several m/z peaks for which the related species assignation is ambiguous. This paper shows how the analysis of the coincident mass-tagged Threshold PhotoElectron Spectra (TPES) together with first principle computations, consisting of the determination of the adiabatic ionization energies and the spectra of some products, may assist products’ identification. The results mostly confirm those previously obtained by photoionization mass spectrometry and gas chromatography, but also allow a more accurate estimation of the 1-pentene/2-pentene mole fraction ratio. Our data also indicate a higher formation of acetone and methyl ethyl ketone than what is predicted by current models, as well as the presence of products that were not previously taken into account, such as methoxyacetylene, methyl vinyl ketone or furanone. The formation of three, four and five membered ring cyclic ethers is confirmed along with linear ketones: 2- and 3-pentanone. A significant general trend in indicating higher amounts of ketones than are indicated by gas chromatography is noted. Finally, TPES of alkenylhydroperoxides are also provided for the first time and constrains on the isomers identification are provided.Lire moins >
Langue :
Anglais
Comité de lecture :
Oui
Audience :
Internationale
Vulgarisation :
Non
Établissement(s) :
Université de Lille
CNRS
CNRS
Équipe(s) de recherche :
PhysicoChimie de la Combustion (PC2)
Date de dépôt :
2020-11-07T18:55:14Z
2020-11-18T14:15:18Z
2020-11-18T14:15:18Z
Fichiers
- PCCP_Manuscript_Review_Lilloa-HAL.pdf
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