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An, Kwangjin
Advanced Nanocatalysis Lab (An Lab)
Research Interests
  • Nanoparticle catalytsts, catalytic activity, selectivity, and stability, strong metal-support interactions, biofuel conversion

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High Structure Sensitivity of Vapor-Phase Furfural Decarbonylation/Hydrogenation Reaction Network as a Function of Size and Shape of Pt Nanoparticles

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Title
High Structure Sensitivity of Vapor-Phase Furfural Decarbonylation/Hydrogenation Reaction Network as a Function of Size and Shape of Pt Nanoparticles
Author
Pushkarev, Vladimir V.Musselwhite, NAn, KwangjinAlayoglu, SSomorjai, GA
Keywords
Pt nanoparticles; Pt/SiO2 catalyst; structure sensitivity; furfural; decarbonylation; hydrogenation
Issue Date
2012-10
Publisher
AMER CHEMICAL SOC
Citation
NANO LETTERS, v.12, no.10, pp.5196 - 5201
Abstract
Vapor-phase transformations of furfural in H 2 over a series of Pt nanoparticles (NPs) with various particle sizes (1.5-7.1 nm size range) and shapes (rounded, cubes, octahedra) encapsulated in poly(vinylpyrrolidone) (PVP) and dispersed on MCF-17 mesoporous silica were investigated at ambient pressure in the 443-513 K temperature range. Furan and furfuryl alcohol (FFA) were two primary products as a result of furfural decarbonylation and hydrogenation reactions, respectively. Under conditions of the study both reactions exhibited structure sensitivity evidenced by changes in product selectivities, turnover rates (TORs), and apparent activation energies (E A's) with Pt particle size and shape. For instance, upon an increase in Pt particle size from 1.5 to 7.1 nm, the selectivity toward FFA increases from 1% to 66%, the TOR of FFA production increases from 1 × 10 -3 s -1 to 7.6 × 10 -2 s -1, and E A decreases from 104 kJ mol -1 to 15 kJ mol -1 (9.3 kPa furfural, 93 kPa H 2, 473 K). Conversely, under the same experimental conditions the decarbonylation reaction path is enhanced over smaller nanoparticles. The smallest NPs (1.5 nm) produced the highest selectivity (96%) and highest TOR values (8.8 × 10 -2 s -1) toward furan formation. The E A values for decarbonylation (∼62 kJ mol -1) was Pt particle size independent. Furan was further converted to propylene via a decarbonylation reaction, but also to dihydrofuran, tetrahydrofuran, and n-butanol in secondary reactions. Furfuryl alcohol was converted to mostly to 2-methylfuran. © 2012 American Chemical Society.
URI
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DOI
10.1021/nl3023127
ISSN
1530-6984
Appears in Collections:
ECHE_Journal Papers
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