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  • 1
    ISSN: 1572-879X
    Keywords: vanadyl pyrophosphate ; partial oxidation of toluene ; in situ spectroscopy ; reactant–catalyst interaction
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract Vanadyl pyrophosphate catalysts were generated by dehydrating VOHPO4·(1/2)H2O at different temperatures and duration of the dehydration procedure. The as-synthesised materials were characterised by X-ray diffractometry, FTIR spectroscopy and temperature-programmed reduction. The prolongation of the formation period at higher temperatures led to improved crystallinity and lower BET surface areas of the vanadyl pyrophosphate specimens and, additionally, a significantly impeded reducibility of the vanadyl sites was observed. The catalytic performance of the samples was tested in the partial oxidation of toluene to benzaldehyde. The obtained results revealed an increasing benzaldehyde selectivity with improved catalyst crystallinity. In situ FTIR and ESR spectroscopy were used to throw more light on the interaction of the toluene–air feed with the surface of the catalyst.
    Type of Medium: Electronic Resource
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  • 2
    ISSN: 1572-9028
    Keywords: ammoxidation ; vanadium phosphate catalysts ; catalyst/feed interaction ; reaction mechanism ; FTIR spectroscopy ; TAP technique ; isotope experiments ; TPD ; TPRS
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract The reaction pathway of the ammoxidation of toluene on (VO)2P2O7 used as catalyst and the interaction of potential intermediates with the pyrophosphate were studied by spectroscopic techniques (FTIR, EPR), temperature-programmed chemisorptions/ reactions (TPD, TPRS) and transient studies such as the temporal analysis of products (TAP) technique. NH3 is chemisorbed on the catalyst surface, forming three different species, i.e., NH 4 + ions located on BrØnsted sites, coordinatively bound NH3 on Lewis sites and NH 2 − groups, presumably P-NH2. Toluene that is probably adsorbed on Lewis sites reacts in a first step to a benzyl radical. A subsequent partial oxidation by interaction of VIV=O groups generates a V...O=CH-C6H5 surface structure. This benzaldehyde-like surface species reacts with adsorbed NH3 according to a Langmuir-Hinshelwood mechanism. TAP experiments on ammonium-containing vanadium phosphates revealed that NH 4 + ions could act as potential N-insertion species. No formation of benzylamine as well as the generation of V=NH surface groups as possible intermediates or N-insertion sites were observed.
    Type of Medium: Electronic Resource
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