期刊
ENERGY & FUELS
卷 36, 期 14, 页码 7608-7616出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.energyfuels.2c01475
关键词
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资金
- National Natural Science Foundation of China (NSFC) [52122608, 51976074]
- Analytical and Testing Centre of Huazhong University of Science and Technology
- Equipment Centre in State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology
Stable free radicals generated during bio-oil pyrolysis are related to bio-oil polymerization and coke structure change. These free radicals have different activation energies, mainly generated from the polymerization of bio-oil.
Thermal-chemical conversion is needed to improve the quality of bio-oil. When bio-oil is heated, it polymerizes to form coke, causing severe problems to its upgrading processes and thus hindering its further utilization. As stable free radicals are generated and attached to coke during the active radical polymerization of bio-oil, figuring out the evolution of stable free radicals is a key to revealing the coke formation mechanisms. In this study, bio-oil pyrolysis was conducted between 300 and 600 degrees C, coupled with in situ electron paramagnetic resonance (EPR) detection. The results indicate that the stable free radicals generated during pyrolysis are related to bio-oil polymerization and coke structure change. In the heating stage, the stable free radicals are generated from the polymerization of bio-oil and the condensation of coke, and the process can be expressed by two first-order kinetics with activation energies of 14.57 and 10.51 kJ/mol, respectively. The aromatic structure stable radicals are generated mainly by the polymerization of bio-oil with an activation energy of 12.66 kJ/mol. In the cooling stage, the free radical reaction would be caused by coke shrinkage, leading to further changes in coke structure.
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