Abstract. The effect of O2 and N2O on alkane reactivity and olefin selectivity in the oxidative dehydrogenation of ethane, propane, n-butane, and iso-butane over highly dispersed VOx species (0.79 V/nm2) supported on MCM-41 has been systematically investigated. For all the reactions studied, olefin selectivity was significantly improved upon replacing O2 with N2O. This is due to suppressing…
Abstract. Time-resolved in situ UV/Vis spectroscopy has been successfully applied for analyzing the reduction degree of highly dispersed VOx (0.4–1.1 V/nm2) species over Ti–Si-MCM-41 (Ti/Si = 0–1.5) materials in the oxidative dehydrogenation of propane (ODP) as well as for deriving the kinetic parameters of reduction (with C3H8) and reoxidation (with O2 and N2O) of these species. This…
Abstract. The mechanism of ammonia oxidation over Pt, Pd, and Rh wires has been investigated in the Temporal Analysis of Products (TAP) reactor at relevant temperatures in industrial ammonia burners. The results of primary (NH3 + O2) and secondary (NH3 + NO) interactions with isotopically labeled ammonia at 1073 K enable to conclude that the overall reaction pathways to NO, N2O, and N2 are …
Abstract. The role of vanadyl and peroxovanadate oxygen species in the oxidative dehydrogenation of propane (ODP) was analyzed by density functional theory (DFT). The dehydrogenation of C3H8 to C3H6 and the oxidation of C3H6 occurred over vanadyl oxygen of VOx species, yielding reduced VOx species. The vanadyl oxygen species were restored via reoxidation of reduced VOx species with O2 and N2O.…
Abstract. A temporal analysis of products (TAP) reactor was used to study relationships between the mechanism of direct N2O decomposition over metal-loaded zeolites and their resulting activity. Rh-ZSM-5 (prepared by incipient wetness) and Fe-ZSM-5 (prepared by liquid-ion exchange) were chosen as prototypic catalysts displaying low (650 K) temperature activity, respectively. Transient studi…