Abstract
1-butene is an important intermediate in combustion of various hydrocarbon fuels and oxygenated biofuels (e.g., butanol). Understanding its oxidation chemistry can help improve ignition and combustion process in advanced engines and provide better emission control. This work addresses a discrepancy between experiments and simulations in 1-butene oxidation at low temperatures, wherein simulations with AramcoMech 3.0 model show greater fuel reactivity than experiments. To further explore 1-butene low temperature reaction pathways from 550 to 910 K, experiments were conducted in three jet-stirred reactors: two coupled to time-of-flight molecular beam mass spectrometers with synchrotron vacuum ultraviolet radiation as the photoionization source, and one coupled to gas chromatography mass spectrometer. Isomeric structure identification, comprehensive species datasets, and reactor cross examinations are provided by the combination of three experiments. The identified isomer-resolved species provide evidence of various 1-butene low temperature reaction pathways. For example, the identification of propanal confirms the Waddington reaction pathway. The kinetic model over-predicts fuel reactivity in the low temperature regime (550–700 K). Updating the rate coefficients of key reactions in the Waddington pathways, e.g., forward and reverse isomerization of hydroxyl-butyl-peroxide to butoxyl-peroxide and Waddington decomposition of butoxyl-peroxide reduces the discrepancies. The role of rate constant updates in each step of the Waddington pathway is evaluated and discussed to provide directions for future model development.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 259-271 |
| Number of pages | 13 |
| Journal | Combustion and Flame |
| Volume | 222 |
| DOIs | |
| State | Published - Sep 10 2020 |
Bibliographical note
KAUST Repository Item: Exported on 2020-10-01Acknowledgements: The research reported in this paper was supported by funding from the King Abdullah University of Science and Technology (KAUST) and the Clean Combustion Research Center (CCRC), and by the National Natural Science Foundation of China (51976208, 91541201). SMS acknowledges support from the KAUST Clean Fuels Consortium (KCFC) and its member companies. BC and HP gratefully acknowledge financial support by the Deutsch Forschungsgemeinschaft within the framework of the collaborative research center SFB/Transregio 129 “Oxyflame”. NH acknowledges support from the U.S. DOE, Office of Science, Office of Basic Energy Sciences. Sandia National Laboratories is a multi-mission laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC. a wholly owned subsidiary of Honeywell International, Inc. for the U.S. DOE National Nuclear Security Administration under contract DE-NA0003525. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. DOE under Contract No. DEAC02-05CH11231.