An experimental and kinetic modeling study on the low-temperature oxidation of oxymethylene ether-2 (OME-2) by means of stabilized cool flames

Ras, Kevin De; Panaget, Thomas; Fenard, Yann; Aerssens, Jeroen; Pillier, Laure; Thybaut, Joris W.; Vanhove, Guillaume

doi:10.1016/j.combustflame.2023.112792

Cited by 5 publications

(15 citation statements)

References 61 publications

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“…At these higher temperatures, OME-derived radicals will not add to molecular oxygen, thereby preventing the formation of cyclic ethers. 31 As such, these temperatures are less relevant in the context of this study.…”

Section: Resultsmentioning

confidence: 96%

“…At higher temperatures, a discrepancy of up to a factor of 3.7 at 1800 K is found between both studies, with the values determined in this work being the lower ones. At these higher temperatures, OME-derived radicals will not add to molecular oxygen, thereby preventing the formation of cyclic ethers . As such, these temperatures are less relevant in the context of this study.…”

Section: Results and Discussionmentioning

confidence: 97%

“…Finally, with the increasing amount of high-level quantum chemical data for OMEs and OME-derived species becoming available in the literature, ,,,,− it would be interesting to compare the estimation methods developed in this work with novel methods, such as machine learning. The performance of kinetic group additivity, which can be seen as a simplified version of machine learning, indicates the potential of machine learning tools such as deep learning.…”

Section: Results and Discussionmentioning

confidence: 99%

“…The incorporated species cover a variety of different functionalities, such as a hydroperoxy group, a methoxy group, a methoxymethoxy group, a hydroxyl group, etc., which are important during the low-temperature oxidation of OMEs. 31 The complete database is listed in Tables S1 and S2 of the Supporting Information. The methodology used for the calculation of the reaction rate coefficients and the development of the different estimation methods are described in the following sections.…”

Section: Methodsmentioning

confidence: 99%

“…For both reaction families, i.e., the unimolecular decomposition of both 4-membered ring and 6-membered ring cyclic ethers, a quantum chemical database, consisting of 34 4-membered ring and 34 6-membered ring cyclic ethers, has been constructed. The incorporated species cover a variety of different functionalities, such as a hydroperoxy group, a methoxy group, a methoxymethoxy group, a hydroxyl group, etc., which are important during the low-temperature oxidation of OMEs . The complete database is listed in Tables S1 and S2 of the Supporting Information.…”

Section: Methodsmentioning

confidence: 99%

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Unimolecular Decomposition of 1,3-Dioxetane and 1,3,5-Trioxane Derivatives: Fast and Accurate Estimation of Kinetic Parameters

Dossche,

De Ras,

Thybaut

et al. 2024

Energy Fuels

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Oxymethylene ethers (OMEs) are a high-potential novel type of e-fuel, which could play an important role in the transition toward a sustainable transportation sector. During the low-temperature oxidation of these OMEs, various cyclic ethers, such as 1,3-dioxetane and 1,3,5-trioxane derivatives, can be formed. However, the current lack of accurate reaction rate coefficients for the unimolecular decomposition of these cyclic ethers has been highlighted as an important obstacle in the development of detailed kinetic models for the low-temperature oxidation of larger OME molecules. In this light, a database with quantum chemical results has been constructed consisting of 34 4-membered ring and 34 6-membered ring cyclic ethers representing important functional groups present during the low-temperature oxidation of OMEs. This database has been used for the development of three estimation methods for the reaction rate coefficients, i.e., rate rules, the Evans−Polanyi relationship, and kinetic group additivity. Balancing performance and complexity, these three methods are currently still the most commonly used estimation methods by automatic kinetic model generation tools. Based upon an assessment of the results, kinetic group additivity was found to be the most accurate method, reaching kinetic accuracy, i.e., a maximum deviation of 1 order of magnitude, for all but one of the 4-membered rings and all but four of the 6-membered ring cyclic ethers. Interactions between the terminal end of a substituent and the ring in combination with the relative stability of different isomers have been proposed to be the main reason for the significant variations between the reaction rate coefficients of the various species. The kinetic parameters can be easily used for the development of detailed kinetic models for larger OMEs based on first principles.

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Section: Resultsmentioning

confidence: 96%

Section: Results and Discussionmentioning

confidence: 97%