Pathway exploration in low-temperature oxidation of a new-generation bio-hybrid fuel 1,3-dioxane |
| |
| Institution: | 1. Institue of Technical Thermodynamics, RWTH Aachen University, 52062, Aachen, Germany;2. Institute for Combustion Technology, RWTH Aachen University, Templergraben 64, 52056 Aachen, Germany;3. Combustion Research Facility, Sandia National Laboratories, Livermore, CA, 94551, USA;1. Institute for Combustion Technology, RWTH Aachen University, Templergraben 64, 52056 Aachen, Germany;2. NST, Institute of Technology for Nanostructures, University of Duisburg-Essen, 47057 Duisburg, Germany;1. Center for Combustion Energy and Department of Energy and Power Engineering, Tsinghua University, Beijing 100084, PR China;2. Key Laboratory for Thermal Science and Power Engineering of MOE, International Joint Laboratory on Low Carbon Clean Energy Innovation, Tsinghua University, Beijing 100084, PR China;3. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, PR China;4. Department of Mechanical and Aerospace Engineering, Princeton University, Princeton, NJ 08544, USA;1. Institute of Engineering Thermophysics, Chinese Academy of Sciences, Beijing, China;2. School of Engineering Science, University of Chinese Academy of Sciences, Beijing, China;3. Combustion Chemistry Centre, School of Biological and Chemical Sciences, Ryan Institute, MaREI, University of Galway, Galway, Ireland;5. State Key Laboratory of Coal Combustion, School of Energy and Power Engineering, Huazhong University of Science and Technology, Wuhan, China;6. Clean Combustion Research Center (CCRC), King Abdullah University of Science and Technology (KAUST), Thuwal, Saudi Arabia;7. J. Mike Walker’66 Department of Mechanical Engineering, Texas A&M University, College Station, TX, USA;8. Chair of High Pressure Gas Dynamics (HGD), Shock Wave Laboratory, RWTH Aachen University, 52056 Aachen, Germany;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 |
| |
| Abstract: | The joint and flexible utilization of renewable electricity, ligno-cellulosic biomass, and/or CO2 point sources to produce so-called bio-hybrid fuels is a promising solution to achieve carbon neutrality while still meeting the energy demand of the transportation sector. One of the new-generation bio-hybrid fuels is 1,3-dioxane. It has a special chemical structure with two oxygen atoms in a six-membered ring. In this work, the low-temperature oxidation of 1,3-dioxane was studied theoretically and experimentally. Potential energy surfaces of the products of the O2 recombination with the three radicals formed from the H-atom abstraction of 1,3-dioxane were calculated at the DLPNO-CCSD(T)/CBS//B2PLYP-D3/cc-pVTZ level. The reaction rate coefficients were calculated with the RRKM/master equation method (T = 500–2000 K, p = 0.01–100 atm). To validate the proposed pathways, low-temperature oxidation experiments of 1,3-dioxane were performed in a jet stirred reactor (JSR) coupled with a synchrotron photon ionization time of flight molecular beam mass spectrometer (T = 590 K, p = 1 bar). Key intermediates in the investigated pathways were captured and identified by the combination of measured photon ionization efficiency curves and calculated ionization energies. Compared to cyclohexane, which has no oxygen in the six-membered ring, 1,3-dioxane has much weaker C-H bonds for the carbon between the two oxygen atoms, thus enabling faster internal H-atom migration from ROO to QOOH. Furthermore, oxidation of 1,3-dioxane tends to favor cyclic ethers + OH (chain propagation) instead of alkenes + HO2 (chain termination), explaining its high reactivity in the low-temperature regime. |
| |
| Keywords: | |
| 本文献已被 ScienceDirect 等数据库收录！ |
|
