Applied Catalysis A: General, Vol.378, No.2, 144-150, 2010
Effect of V in La2NixV1-xO4+delta on selective oxidative dehydrogenation of propane
In this study, non-stoichiometric redox compounds such as La2NiO4+delta, La2Ni0.95V0.05O4.07+delta and La2Ni0.9V0.1O4.15+delta have been tested as oxidants in selective oxidation of propane, in order to judge the suitability of these materials for a dense membrane reactor for selective propane oxidation. Reducibility of the samples has been investigated using temperature programmed reduction in H-2/Ar flow. The catalysts' activity and selectivity at 550 degrees C have been investigated employing sequential pulses of diluted propane over the oxides. Pulsing with propane induces step-by-step reduction of the oxide: consequently, the activity of remaining oxygen decreases with the number of pulses, affecting the products distribution. It is observed that at 550 degrees C on oxidized catalysts CO2 and H2O are the main products and the selectivity towards propylene is very low. At a certain reduction level, obtained after pulse 8 in our experiments, the production of CO2 stopped without changing the amount of C3H6 produced. At this stage, also CH4 and C2H4 are being formed. V-doped catalysts have shown a constant level of C3H6 production within a broad window of oxidation degree, while the performance of La2NiO4+delta, catalyst deteriorated drastically after just a few pulses. CO, CH 4 and coke deposits are formed with La2NiO4+delta, caused by the formation of metallic Ni. Vanadium is able to prevent this phenomenon, thus drastically broadening the window of selective oxidation of propane. (C) 2010 Elsevier B.V. All rights reserved.