New insights into the oxidation chemistry of pyrrole,an N-containing biomass tar component |
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| Institution: | 1. Institute for Combustion Technology, RWTH Aachen University, Templergraben 64, 52056 Aachen, Germany;2. King Abdullah University of Science and Technology (KAUST), Clean Combustion Research Center, Thuwal, Saudi Arabia;3. CRECK Modelling Lab, Department of Chemistry, Materials, and Chemical Engineering “Giulio Natta”, Politecnico di Milano, Piazza Leonardo da Vinci 32, 20133 Milan, Italy;4. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, China;5. Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China;6. Chair of Technical Thermodynamics, RWTH Aachen University, Schinkelstraße 8, 52062 Aachen, Germany;7. State Key Laboratory of Fire Science, University of Science and Technology of China, Hefei, Anhui 230026, China;1. Combustion Research Facility, Sandia National Laboratories, Livermore, CA 94551, USA;2. Lawrence Livermore National Laboratory, Livermore, CA 94551, USA;3. Institute for Combustion Technology, RWTH Aachen University, 52056 Aachen, Germany;4. Combustion Chemistry Centre, Ryan Institute, MaREI, National University of Ireland, Galway, Ireland;5. Department of Chemistry, University of Helsinki, FI-00560 Helsinki, Finland;6. Physikalisch-Technische Bundesanstalt, Bundesallee 100, 38116 Braunschweig, Germany;7. Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL 60439, USA;8. National Synchrotron Radiation Laboratory, USTC, Hefei, Anhui 230029, PR China;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. Institute of Engineering Thermophysics, Chinese Academy of Sciences, Beijing 100190, China;2. University of Chinese Academy of Sciences, Beijing 100049, China;3. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, China;4. Key Laboratory for Power Machinery and Engineering of MOE, Shanghai Jiao Tong University, Shanghai 200240, China;1. Center for Combustion Energy and Key Laboratory for Thermal Science and Power Engineering of MOE, Tsinghua University, Beijing 100084, China;2. Combustion Research Facility, Sandia National Laboratories, Livermore, CA 94551, United States;3. Institute for Combustion Technology, RWTH Aachen University, 52056 Aachen, Germany |
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| Abstract: | Pyrrole, the smallest molecule with a nitrogen atom in the heterocycle ring, is an important tar component from coal and nitrogen-rich biomass devolatilization. Understanding the combustion chemistry of pyrrole can help to elucidate the pollutant formation chemistry from fuel nitrogen, thus enabling cleaner biomass energy utilization technologies. Experimental measurements were performed in a jet stirred reactor coupled with time of flight molecular beam mass spectrometry using synchrotron vacuum ultraviolet beam as photon ionization source, and gas chromatography-mass spectrometry to provide comprehensive measurements of 31 species including nine C4 and C5 N-containing compounds. Based on the evidence from the experiments and aiming to improve the kinetic model performance, possible formation routes are proposed with OH addition as the entrance reaction. Reaction rate coefficients for the OH addition channel as well as those for key H-atom abstraction reactions (H, OH, CH3, and HO2) were calculated by quantum chemical methods and updated in the model. The updated model can qualitatively predict the identified C4 N-containing species and perform reasonably well for a large set of experimental data considered for validation, overall improving the performance of the previous model. The influence of the investigated reactions on the predictions of fuel reactivity and pollutant formation motivates further investigations of N-containing fuel chemistry. |
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