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  • 1
    ISSN: 1572-879X
    Keywords: Faujasite X hosted rhodium ; rhodium particle size ; IR-spectroscopy ; TEM ; CO hydrogenation
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract Different metal dispersions of Na-faujasite X hosted rhodium were generated and characterized by transmission electron microscopy (TEM) and IR-spectroscopy. CO hydrogenation has been studied over these Rh/NaX-zeolite catalysts. The finer rhodium dispersion with a mean particle size of 1–2 nm shows a higher selectivity towards oxygenates (methanol, ethanol and dimethyl ether) as compared to the coarser dispersion (4–5 nm), where nearly exclusively methane and higher hydrocarbons are formed.
    Type of Medium: Electronic Resource
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  • 2
    ISSN: 1572-879X
    Keywords: faujasite-hosted rhodium ; in situ FTIR spectroscopy ; CO hydrogenation ; rhodium dispersion ; methanol selectivity
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract In situ FTIR spectroscopy has been applied to study the reason of the different selectivity behaviour of rhodium in the CO hydrogenation reaction in dependence on the different particle size. Several forms of molecularly adsorbed CO are observed, such as linearly- and bridgedbonded CO on metallic rhodium as well as dicarbonyl species with Rh(I) centres formed by oxidation of Rh(0) with protons in presence of CO. Furthermore, non-reactive formate, acetate, and carbonate species are produced as side products of the reaction. The higher selectivity to oxygenates, particularly to methanol, is explained by the existence of multiple-bonded CO present only on small rhodium crystallites. The multiple-bonded CO formed at low temperatures is converted at higher temperatures to the highly reactive formyl species, which is hydrogenated to methanol.
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  • 3
    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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