NDLI: Ligand and Ensemble Effects in Bimetallic NiFe Phosphide Catalysts for the Hydrodeoxygenation of 2-Methyltetrahydrofuran

Content Provider	Springer Nature Link
Author	Cho, Ara Shin, Jieun Takagaki, Atsushi Kikuchi, Ryuji Oyama, S. Ted
Copyright Year	2012
Abstract	A series of supported nickel–iron phosphide catalysts were used to study the hydrodeoxygenation (HDO) of 2-methyltetrahydrofuran (2-MTHF), a model compound for biomass-derived pyrolysis oil. The catalysts were prepared by incipient wetness impregnation of the active components onto potassium ion-exchanged USY zeolites followed by temperature-programmed reduction. The samples were denoted as Ni$_{2}$P/KUSY, NiFeP(3:1)/KUSY, NiFeP(1:1)/KUSY, NiFeP(1:3)/KUSY, and FeP/KUSY, where the numbers in parenthesis are the Ni:Fe molar ratios. The results of the studies can be understood from ensemble and ligand effects. X-ray diffraction analysis indicated the presence of alloys in the mixed composition samples, and this was supported by CO chemisorption and infrared measurements. Uptakes of CO decreased as the iron content increased, suggesting that iron present on the surface of the catalysts blocked chemisorption sites. Fourier transform infrared (FTIR) measurements showed a single peak for linearly adsorbed CO whose intensity decreased with Fe content, in agreement with the uptake results. Moreover, the FTIR peak shifted monotonically consistent with a ligand effect in an alloy formed in the Ni$_{2}$P and FeP particles. The reactivity in 2-MTHF HDO was studied at 250–325 °C and 0.5 MPa and it was found that the conversion was highest for the Ni$_{2}$P/KUSY sample and decreased steadily with Fe content. However, the turnover frequency did not change significantly, indicating that the rate-determing step was activation of 2-MTHF on single Ni sites. The selectivity at low conversion (3 %) changed from mostly n-pentane and n-butane for Ni$_{2}$P/KUSY to mostly 1-pentanol for the iron-containing samples, suggesting that in subsequent steps an ensemble effect was operational with the iron influencing the reaction chemistry. At high conversion (70 %) all the samples produced mostly n-pentane and n-butane.
Starting Page	969
Ending Page	980
Page Count	12
File Format	PDF
ISSN	10225528
Journal	Topics in Catalysis
Volume Number	55
Issue Number	14-15
e-ISSN	15729028
Language	English
Publisher	Springer US
Publisher Date	2012-09-05
Publisher Place	Boston
Access Restriction	One Nation One Subscription (ONOS)
Subject Keyword	Hydrodeoxygenation 2-Methyltetrahydrofuran Phosphides Ni$_{2}$P and FeP KUSY supports Pharmacy Catalysis Industrial Chemistry/Chemical Engineering Characterization and Evaluation of Materials Physical Chemistry
Content Type	Text
Resource Type	Article
Subject	Chemistry Catalysis

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