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An, Kwangjin
Advanced Nanocatalysis Lab (An Lab)
Research Interests
  • Nanoparticle catalytsts, catalytic activity, selectivity, and stability, strong metal-support interactions, CO2 utilization, biomass conversion, Plastic Up-cycling

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Designed Catalysts from Pt Nanoparticles Supported on Macroporous Oxides for Selective Isomerization of n-Hexane

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Title
Designed Catalysts from Pt Nanoparticles Supported on Macroporous Oxides for Selective Isomerization of n-Hexane
Author
An, KwangjinS AlayogluN MusselwhiteK NaGA Somorjai
Keywords
Catalysts; Gasoline refining; Hexane; Hydrocarbon refining; Isomerization; Isomers; Nanoparticles; Niobium; Photoelectrons; Platinum; Tantalum; Tantalum oxides; X ray diffraction; X ray photoelectron spectroscopy
Issue Date
2014-04
Publisher
AMER CHEMICAL SOC
Citation
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.136, no.19, pp.6830 - 6833
Abstract
Selective isomerization toward branched hydrocarbons is an important catalytic process in oil refining to obtain high-octane gasoline with minimal content of aromatic compounds. Colloidal Pt nanoparticles with controlled sizes of 1.7, 2.7, and 5.5 nm were deposited onto ordered macroporous oxides of SiO2, Al2O3, TiO2, Nb2O5, Ta2O5, and ZrO2 to investigate Pt size- and support-dependent catalytic selectivity in n-hexane isomerization. Among the macroporous oxides, Nb2O5 and Ta2O5 exhibited the highest product selectivity, yielding predominantly branched C-6 isomers, including 2- or 3-methylpentane, as desired products of n-hexane isomerization (140 Torr n-hexane and 620 Torr H-2 at 360 degrees C). In situ characterizations including X-ray diffraction and ambient-pressure X-ray photoelectron spectroscopy showed that the crystal structures of the oxides in Pt/oxide catalysts were not changed during the reaction and oxidation states of Nb2O5 were maintained under both H-2 and O-2 conditions. Fourier transform infrared spectra of pyridine adsorbed on the oxides showed that Lewis sites were the dominant acidic site of the oxides. Macroporous Nb2O5 and Ta2O5 were identified to play key roles in the selective isomerization by charge transfer at Pt-oxide interfaces. The selectivity was revealed to be Pt size-dependent, with improved isomer production as Pt sizes increased from 1.7 to 5.5 nm. When 5.5 nm Pt nanoparticles were supported on Nb2O5 or Ta2O5, the selectivity toward branched C-6 isomers was further increased, reaching ca. 97% with a minimum content of benzene, due to the combined effects of the Pt size and the strong metal-support interaction.
URI
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DOI
10.1021/ja5018656
ISSN
0002-7863
Appears in Collections:
ECHE_Journal Papers
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JACS 2014,136,6830, Designed Catalysts from Pt NPs Supported on M-Oxides for Selective Isomerization of n-Hexane.pdf Download

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