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This study compares different modes of limonene oxidation (ozonolysis, photooxidation and cool flame) on the basis of review articles and experimental results. Although the oxidation conditions are totally different, the results obtained present great similarities on the nature of the products, but also specificities related to autooxidation such as the presence of ketohydroperoxides.
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https://doi.org/10.5194/acp-2020-1070
https://doi.org/10.5194/acp-2020-1070

  08 Dec 2020

08 Dec 2020

Review status: this preprint is currently under review for the journal ACP.

On the similarities and differences between the products of oxidation of hydrocarbons under simulated atmospheric conditions and cool-flames

Roland Benoit1, Nesrine Belhadj1,2, Maxence Lailliau1,2, and Philippe Dagaut1 Roland Benoit et al.
  • 1CNRS-INSIS, ICARE, Orléans, France
  • 2Université d'Orléans, Orléans, France

Abstract. Whereas the kinetics of oxidation of limonene has been extensively studied and mechanisms for its oxidation by OH and/or ozone have been proposed, more studies are required for better understanding its oxidation pathways. The oxidation of limonene-oxygen-nitrogen mixtures was studied using a jet-stirred reactor at elevated temperature and atmospheric pressure. Samples of the reacting mixtures were collected and analyzed by high resolution mass spectrometry (Orbitrap) after direct injection or after separation by reverse-phase ultra-high-pressure liquid chromatography and soft ionization by (+/−) HESI and (+/−) APCI. The results indicate that among the 1138 detected products, many oxygenates found in earlier studies of limonene oxidation by OH and/or ozone are also produced under the present conditions. Other highly oxygenated products and oligomers were also detected in the present work. The results are discussed in terms of reaction pathways involving the initial formation of peroxy radicals, isomerization reactions yielding keto-hydroperoxides and other oxygenated intermediates and products up to C25H32O17. The possible occurrence of the Waddington mechanism and of the Korcek mechanism are also discussed. The present work demonstrates similarities between the oxidation products and oxidation pathways of limonene under simulated atmospheric conditions and in those encountered during the self-ignition of hydrocarbons at low temperatures, which should stimulate future interactions between communities of atmospheric chemistry and combustion chemistry to improve current chemical models.

Roland Benoit et al.

 
Status: open (until 26 Feb 2021)
Status: open (until 26 Feb 2021)
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Roland Benoit et al.

Roland Benoit et al.

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Short summary
This study compares different modes of limonene oxidation (ozonolysis, photooxidation and cool flame) on the basis of review articles and experimental results. Although the oxidation conditions are totally different, the results obtained present great similarities on the nature of the products, but also specificities related to autooxidation such as the presence of ketohydroperoxides.
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