On the low-temperature chemistry of 1,3-butadiene |
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| Affiliation: | 1. State Key Laboratory of Coal Combustion, School of Energy and Power Engineering, Huazhong University of Science and Technology, Wuhan, China;2. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui, China;3. Combustion Chemistry Centre, School of Biological and Chemical Sciences, Ryan Institute, MaREI, University of Galway, Galway, H91 TK33, Ireland;1. Key Laboratory for Power Machinery and Engineering of MOE, School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China;2. Institute of Thermal Engineering, Technische Universität Bergakademie Freiberg, Freiberg D-09599, Germany;1. State Key Laboratory of Fire Science, University of Science and Technology of China, Hefei 230026, China;2. Dalian National Laboratory for Clean Energy, Dalian 116023, China;1. Combustion Chemistry Centre, School of Biological and Chemical Sciences, Ryan Institute, MaREI, University of Galway, University Road, Galway H91 TK33, Ireland;2. Shell Global Solutions, (Deutschland) Hohe-Schaar-Straße 36, 21107 Hamburg, Germany;3. Shell Global Solutions (UK), Shell Centre London, London SE1 7NA, United Kingdom;1. School of Energy and Power Engineering, Beihang University, Beijing 100191, China;2. Department of Mechanical Engineering, University of Connecticut, Storrs, CT 06269, United States;3. Research Institute of Petroleum Processing, Sinopec, 18 Xueyuan Road, Haidian District, Beijing 100083, China;4. School of Astronautics, Beihang University, Beijing 100191, China;5. Combustion Chemistry Centre, School of Chemistry, Ryan Institute, National University of Ireland, Galway, Galway H91TK33, Ireland;1. Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, 230026, PR China;2. Display Asia Process and Product Development, Corning (Wuhan) Co. Ltd., Wuhan, Hubei, 430040, PR China;3. College of Information Engineering, China Jiliang University, Hangzhou, Zhejiang, 310018, PR China;4. Key Laboratory for Microstructural Material Physics of Hebei Province, School of Science, Yanshan University, Qinhuangdao, Hebei, 066004, PR China;1. Materials Science Division, Lawrence Livermore National Laboratory, Livermore, CA 94551, USA;2. Combustion Chemistry Centre, School of Chemistry, Ryan Institute, MaREI, National University of Ireland, Galway, Ireland;3. Department of Mechanical Engineering, University of Colorado Boulder, Boulder, CO 80309, USA |
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| Abstract: | In this paper, species versus temperature profiles were measured during the oxidation of 1,3-butadiene in a jet-stirred reactor (JSR) at 1 atm, at different equivalence ratios (φ = 0.5, 1.0 and 2.0), in the temperature range 600 – 1020 K. Both synchrotron vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS) and gas chromatography (GC) methods were used to analyze the species. The experimental results show that a large proportion of the products are aldehydes (formaldehyde, acetaldehyde, acrolein, etc.) and ketenes (ketene, methyl-ketene), with acrolein being one of the major products. Moreover, furan, 1,3-cyclopentadiene and benzene are also present as intermediates in significant amounts. The reaction pathways leading to the formation of these species are discussed in detail. A new detailed mechanism, NUIGMech1.3, was developed to simulate these new data as well as other experimental data available in the literature. The validation results indicate that quantum calculations are also needed to explore the formation of some important species formed in the oxidation of 1,3-butadiene. Overall, the new 1,3-butadiene mechanism agrees well with various experimental data in the low- to high-temperature regimes and at different pressures. Flux and sensitivity analyses show that 1,3-butadiene shares some common reaction chemistry pathways with 1- and 2-butene via Ḣ atom and HȮ2 radical addition to the C = C double bond in 1,3-butadiene, reactions which are important for both systems. The low temperature chemistry of 1,3-butadiene is mainly controlled by the reaction pathways of ȮH radical addition to the C = C double bond of the fuel molecule. The 1-buten-4-ol-3-yl radicals so formed subsequently add to O2 and react via the Waddington mechanism, which is important in accurately simulating the oxidation and auto-ignition of 1,3-butadiene at engine relevant conditions. |
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| Keywords: | SVUV-PIMS Kinetics modeling |
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