期刊
CHEMCATCHEM
卷 10, 期 10, 页码 2219-2231出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.201702001
关键词
catalyst deactivation; hydrodeoxygenation; organosilanes; support surface polarity; tetraethyl orthosilicate
资金
- European Commission [604307]
- ERC Consolidator Grant (LIGNINFIRST) [725762]
- Royal Society
- EPSRC [EP/K000616/2]
Hydrodeoxygenation (HDO) of lignocellulose-derived pyrolysis oils offers an option to produce fuel substitutes. However, catalyst deactivation and stability constitute a significant issue. Herein, the dependence of stability and activity of Ni2P/SiO2 HDO catalysts on the support surface polarity is addressed in detail. The support surface polarity was adjusted by copolymerizing tetraethyl orthosilicate (TEOS) with different types and amounts of organosilanes by a sol-gel process in the presence of nickel nitrate and citric acid. After thermal treatment under an inert atmosphere, Ni/SiO2 precursors were formed. They were converted into Ni2P/SiO2 catalysts by using NaH2PO2 as a PH3 source. The catalyst surface polarity was characterized by inverse gas chromatography measurements of the free energy of methanol adsorption, and specific and dispersive surface energies derived from polar and nonpolar probe molecule adsorption. The correlation between catalyst performance and support surface polarity indicates that, to prevent deactivation of the catalyst by water under reaction conditions, the affinity of the support towards polar substances must be decreased below a threshold value.
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