Please use this identifier to cite or link to this item: http://dx.doi.org/10.14279/depositonce-5268
Main Title: Anomalous reactivity of supported V2O5 nanoparticles for propane oxidative dehydrogenation: influence of the vanadium oxide precursor
Author(s): Carrero, Carlos A.
Keturakis, Christopher J.
Orrego, Andres
Schomäcker, Reinhard
Wachs, Israel E.
Type: Article
Language Code: en
Abstract: The oxidative dehydrogenation (ODH) of propane to propylene by supported vanadia catalysts has received much attention in recent years, but different reactivity trends have been reported for this catalytic reaction system. In the present investigation, the origin of these differing trends are investigated with synthesis of supported V/SiO2, V/TiO2, and V/Al2O3 catalysts prepared with three different vanadium oxide precursors (2-propanol/vanadyl triisopropoxide [VO(O-Pri)3] (VTI), oxalic acid/ammonium metavanadate [NH4VO3] (AMV), and toluene/vanadyl acetylacetonate [VO(C5H7O2)2] (VAA)) in order to elucidate the influence of the precursor on supported vanadia phase and propane ODH activity. In situ Raman spectroscopy revealed that the choice of vanadium precursor does not affect the dispersion of the supported vanadium oxide phase below 4 V nm−2 (0.5 monolayer coverage), where only isolated and oligomeric surface VO4 species are present, and only the AMV precursor favors crystalline V2O5 nanoparticle (NP) formation below monolayer coverage (8 V nm−2). The propane ODH specific reactivity trend demonstrated that there is no significant difference in TOF for the isolated and oligomeric surface VO4 sites. Surprisingly, V2O5 NPs in the ∼1–2 nm range exhibit anomalously high propane ODH TOF values for the supported vanadia catalysts. This was found for all supported vanadium oxide catalysts examined. This comparative study with different V-precursors and synthesis methods and oxide supports finally resolves the debate in the catalysis literature about the dependence of TOF on the surface vanadium density that is related to the unusually high reactivity of small V2O5 NPs.
URI: http://depositonce.tu-berlin.de/handle/11303/5648
http://dx.doi.org/10.14279/depositonce-5268
Issue Date: 2013
Date Available: 24-Jun-2016
DDC Class: 540 Chemie und zugeordnete Wissenschaften
Sponsor/Funder: DFG, SFB 546, Struktur, Dynamik und Reaktivität von Übergangsmetalloxid-Aggregaten
Usage rights: Terms of German Copyright Law
Journal Title: Dalton transactions : a journal of inorganic chemistry, including bioinorganic, organometallic, and solid-state chemistry
Publisher: Royal Society of Chemistry
Publisher Place: Cambridge
Volume: 42
Issue: 35
Publisher DOI: 10.1039/c3dt50611h
Page Start: 12644
Page End: 12653
EISSN: 1477-9226
Notes: Dieser Beitrag ist mit Zustimmung des Rechteinhabers aufgrund einer (DFG geförderten) Allianz- bzw. Nationallizenz frei zugänglich.
This publication is with permission of the rights owner freely accessible due to an Alliance licence and a national licence (funded by the DFG, German Research Foundation) respectively.
Appears in Collections:Technische Universität Berlin » Fakultäten & Zentralinstitute » Fakultät 2 Mathematik und Naturwissenschaften » Institut für Chemie » Publications

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