Gas-phase dehydration of tetrahydrofurfuryl alcohol to dihydropyran over γ-Al2O3
Autor: | Daniel J. McClelland, Kevin J. Barnett, Dongting Zhao, George W. Huber, Guozhu Liu, Ling Li |
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Rok vydání: | 2019 |
Předmět: |
Reaction mechanism
Dihydropyran Process Chemistry and Technology Inorganic chemistry 02 engineering and technology 010402 general chemistry 021001 nanoscience & nanotechnology medicine.disease 01 natural sciences Catalysis 0104 chemical sciences law.invention chemistry.chemical_compound chemistry law Desorption medicine Calcination Dehydration Isopropylamine 0210 nano-technology Selectivity General Environmental Science |
Zdroj: | Applied Catalysis B: Environmental. 245:62-70 |
ISSN: | 0926-3373 |
DOI: | 10.1016/j.apcatb.2018.12.039 |
Popis: | Gas-phase dehydration of tetrahydrofurfuryl alcohol (THFA) to 3,4-2H-dihydropyran (DHP) was studied over solid acid catalysts. A γ-Al2O3 catalyst resulted in 90% DHP yield from THFA. The γ-Al2O3 deactivated due to solid coke formation but was nearly fully re-generable upon a high temperature calcination step (only 2.5% activity loss after 3rd regeneration). The high catalytic activity and selectivity of γ-Al2O3 was correlated to its high Lewis to Brϕnsted acid site ratio, as confirmed by ammonia temperature-programmed desorption (NH3-TPD) and isopropylamine temperature-programmed desorption (IPA-TPD). Based on isotopic-labelling studies, a reaction mechanism was proposed in which THFA initially dehydrates into a carbenium intermediate prior to Wagner-Meerwien rearrangement into DHP. A kinetic model of THFA dehydration over γ-Al2O3 was developed according to kinetic experimental data. The best-fit model suggested the rate-determining step was the surface reaction of adsorbed THFA dissociating into adsorbed DHP and water. |
Databáze: | OpenAIRE |
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