Jet-Stirred Reactor Study of Low-Temperature Neopentane Oxidation: A Combined Theoretical, Chromatographic, Mass Spectrometric, and PEPICO Analysis
| Autor: | Luc-Sy Tran, Olivier Herbinet, Gustavo García, Philippe Arnoux, Majdi Hochlaf, Laurent Nahon, Zhandong Wang, Hans-Heinrich Carstensen, Guillaume Vanhove, Jérémy Bourgalais, Frédérique Battin-Leclerc, Janney Debleza, Binzhi Liu |
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| Přispěvatelé: | Laboratoire Réactions et Génie des Procédés (LRGP), Centre National de la Recherche Scientifique (CNRS)-Université de Lorraine (UL), Department of chemical engineering INA University of Zaragoza, Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Physicochimie des Processus de Combustion et de l’Atmosphère - UMR 8522 (PC2A), Université de Lille-Centre National de la Recherche Scientifique (CNRS), National Synchrotron Radiation Laboratory (NSRL), University of Science and Technology of China [Hefei] (USTC), COSYS-LISIS, Université Gustave Eiffel, IFSTTAR, Marne-la-Vallée F-77454, France (COSYS-LISIS), Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), University of Zaragoza - Universidad de Zaragoza [Zaragoza], Laboratoire Instrumentation, Simulation et Informatique Scientifique (COSYS-LISIS), Université Gustave Eiffel, Université de Lille, CNRS, Laboratoire Réactions et Génie des Procédés [LRGP], Synchrotron SOLEIL [SSOLEIL], Physicochimie des Processus de Combustion et de l'Atmosphère (PC2A) - UMR 8522, National Synchrotron Radiation Laboratory [NSRL], Laboratoire Instrumentation, Simulation et Informatique Scientifique [COSYS-LISIS], Centre National de la Recherche Scientifique (CNRS)-Université de Lille |
| Jazyk: | angličtina |
| Rok vydání: | 2021 |
| Předmět: |
Kinetic modeling
General Chemical Engineering Gadolinium Energy Engineering and Power Technology Nanoparticle chemistry.chemical_element Terbium 010402 general chemistry Photochemistry 01 natural sciences 7. Clean energy chemistry.chemical_compound Succinimide [CHIM.ANAL]Chemical Sciences/Analytical chemistry 0103 physical sciences Organic reactions Oxidation Photosensitizer Ions Chromatography 010304 chemical physics Singlet oxygen Porphyrin 0104 chemical sciences Fuel Technology Neopentane chemistry |
| Zdroj: | Sustainable Energy & Fuels Sustainable Energy & Fuels, Royal Society of Chemistry, 2021, 13 (26), pp.30337-30349. ⟨10.1021/acs.energyfuels.1c02080⟩ Sustainable Energy & Fuels, 2021, 35 (23), pp.19689-19704. ⟨10.1021/acs.energyfuels.1c02080⟩ |
| ISSN: | 2398-4902 |
| DOI: | 10.1021/acs.energyfuels.1c02080⟩ |
| Popis: | International audience; The oxidation of neopentane was studied in jet-stirred reactors at atmospheric pressure over a temperature range 500–850 K and ϕ = 0.5. The products were analyzed with chromatographic, mass spectrometric, and photoelectron spectroscopic setups complemented with theoretical calculations. This combination provides a comparison of photo-ionization mass spectrometry and gas chromatography for the quantification of mole fractions and highlights the relevant differences between them, while mass-tagged photoelectron spectroscopy sheds light onto the isomeric distribution. The new data and corresponding analyses are expected to provide valuable guidance for an extension of the kinetic model and the choice of experimental methods. The main first and second O2-addition products were observed in agreement with the literature (e.g., 3,3-dimethyloxetane, acetone, isobutene, and γ-ketohydroperoxide). The simulated mole fractions of the products using a literature kinetic model were compared to the experimental results. Even though the kinetic model has been validated previously, significant discrepancies between the measured and simulated mole fractions of 2-methylpropanal and methacrolein, two fuel-specific low-temperature oxidation products, were found. Furthermore, some experimentally observed species related to γ-ketohydroperoxide decomposition were not predicted indicating that the model is incomplete. The detection of 2-methylpropanal and formic acid highlighted the importance of the Korcek-type pathway. |
| Databáze: | OpenAIRE |
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