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Low temperature mechanism for the formation of polycyclic aromatic hydrocarbons from the pyrolysis of cellulose
Affiliation:1. Colorado School of Mines, 1500 Illinois Street, Golden, CO, USA;2. National Renewable Energy Laboratory, 15013 Denver West Pkwy, Golden, CO, USA;1. LRGP, CNRS, Université de Lorraine, 1 rue Grandville, 54000 Nancy, France;2. ICS, CNRS, Université de Strasbourg, 1 rue Blaise Pascal BP 296 R8, 67008 Strasbourg Cedex, France;3. IS2M, CNRS, Université de Haute Alsace, 15, rue Jean Starcky BP 2488, 68057 Mulhouse Cedex, France;4. LERMAB, Université de Lorraine, BP239, 54506 Vandoeuvre les Nancy Cedex, France;1. School of Environmental Science and Engineering/State Key Lab of Engines, Tianjin Engineering Center of Biomass-derived Gas and Oil, Key Laboratory of Efficient Utilization of Low and Medium Grade Energy (Ministry of Education), Tianjin University, Tianjin, 300072, China;2. School of Civil Engineering, University of Science and Technology Liaoning, Liaoning Anshan, 114051, China;3. School of Science, Tibet University, No.36 Jiangsu Street, Lhasa, 850012, Tibet Autonomous Region, China;4. Guangzhou Institute of Energy Conversion Guangzhou, Guangdong, 510640, China;5. State Key Laboratory of Multiphase Flow in Power Engineering (SKLMF), Xi''an Jiaotong University, 28 Xianning West Road, Xi''an, 710049, China
Abstract:The formation of polycyclic aromatic hydrocarbons (PAHs) from the pyrolysis of cellulose over the temperature range of 300–650 °C has been investigated. Detectable amounts (microgram per gram) of 2–4 ring PAHs were observed at and above 400 °C. Benzo[a]pyrene and benz[a]anthracene were observed at and above 500 °C. Changing the gas phase residence time from 2 to 18 s and the sample size from 200 to 500 mg did not significantly affect the yields of PAHs formed over this low temperature range. The addition of oxygen to the carrier gas stream significantly reduced the yields of PAHs. The pathway to PAH formation in the 300–650 °C temperature range is believed to proceed via the carbonization process where the solid residue undergoes a chemical transformation and rearrangement to give a more condensed polycyclic aromatic structure. The evolution profiles of PAHs from the solid residue suggests that smaller 2–3 ring PAHs evolve first and pass through a maximum at a slightly lower temperature than the larger 4–5 ring PAHs. The yields of PAHs obtained from the pyrolysis of d-glucose and sucrose are comparable to those obtained from cellulose.
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