期刊
JOURNAL OF CATALYSIS
卷 311, 期 -, 页码 17-27出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2013.11.002
关键词
Nickel phosphide; Hydrodeoxygenation; 2-Methyltetrahydrofuran; Reaction network; Langmuir-Hinshelwood kinetics
资金
- Development of Next-generation Technology for Strategic Utilization of Biomass Energy of New Energy and Industrial Technology Development Organization (NEDO), Japan
- US Department of Energy, Office of Basic Energy Sciences [DE-FG02-963414669]
- Grants-in-Aid for Scientific Research [26289301] Funding Source: KAKEN
Bio-oil obtained by the pyrolysis of woody biomass contains many oxygenated organic compounds which degrade the product quality and make necessary upgrading for its use as a liquid fuel. Hydrodeoxygenation (HDO) is a catalytic hydrotreating process for the removal of the problematic oxygen functionalities and is promising for bio-oil upgrading. In this work, 2-methyltetrahydrofuran (2-MTHF) was chosen as a model oxygenated compound, and its HDO reaction mechanism was studied on a silica-supported nickel phosphide catalyst (Ni2P/SiO2) at a medium pressure of 0.5 MPa. The temperature dependency of the catalyst activity was determined and it was found that at 350 degrees C Ni2P/SiO2 showed 100% conversion and 85% selectivity to n-pentane, with higher oxygen removal activity and less C C bond cracking activity than commercial noble metal Ru/C and Pd/Al2O3 catalysts based on the same amount of active sites. A contact time study allowed the determination of a reaction sequence for 2-MTHF HDO on Ni2P/SiO2 and it was found that C-O bond cleavage of the furanic ring to generate either 2-pentanone or 1-pentanal was the rate-determining step. This was followed by hydrogen transfer steps to produce oxygen free compounds, n-pentane or n-butane. A partial pressure analysis of 2-MTHF and H-2 was consistent with a rate equation derived using a Langmuir-Hinshelwood (L-H) mechanism. This suggested that adsorption of 2-MTHF and hydrogen occurred competitively and that these-species reacted on the Ni2P/SiO2 surface. Although high partial pressure of H-2 was favorable for hydrogenation, too much H-2 competed with 2-MTHF adsorption, which caused lower conversion. (C) 2013 Elsevier Inc. All rights reserved.
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