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- W4256179660 abstract "The kinetics of liquid-phase hydrogenation of citral (3,7-dimethyl-2,6-octadienal) on Pt/TiO2 catalysts were studied between 298–423 K and 7–21 atm H2 and compared to those reported earlier for Pt/SiO2 catalysts. The kinetic data were shown to be free of transport limitations by application of the Madon–Boudart test and the Weisz–Prater criterion. Near zero- and first-order kinetics were observed for the initial rate of citral hydrogenation over the Pt/TiO2-LTR (Tred=473K) and Pt/SiO2 catalysts with respect to citral concentration and hydrogen pressure, respectively. In contrast, each dependency dropped by about one order with Pt/TiO2-HTR (Tred=773K) catalysts as they were negative first-order on citral concentration and near zero-order on hydrogen pressure. Furthermore, the initial rates over Pt/TiO2-LTR and Pt/SiO2 exhibited an activity minimum as temperature increased whereas conventional Arrhenius behavior was exhibited by Pt/TiO2-HTR with an activation energy of 18 kcal/mol. Pt/TiO2-LTR and HTR catalysts initially exhibited 90% selectivity to the unsaturated alcohol as compared to 40% for hydrogenation over Pt/SiO2. Metal–support interactions (MSI) resulted in a dramatic enhancement in specific activity at 373 K, 20 atm H2 and 1 M citral in hexane as Pt/TiO2-HTR exhibited a turnover frequency of 1.0 compared to 0.02 s−1 for Pt/TiO2-LTR and 0.004 s−1 for Pt/SiO2. The reaction kinetics with Pt/TiO2-HTR in the differential conversion regime were described by a conventional Langmuir–Hinshelwood model assuming quasi-equilibrium for reactant adsorption, competitive adsorption between citral and hydrogen, and addition of the first H atom as the rate determining step. The reaction rate at higher conversions was modeled by invoking a decarbonylation reaction similar to that proposed earlier for this reaction over Pt/SiO2 catalysts to explain any observed deactivation." @default.
- W4256179660 created "2022-05-12" @default.
- W4256179660 date "1973-04-01" @default.
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- W4256179660 doi "https://doi.org/10.1016/0021-9517(73)90194-2" @default.
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