Catalysis Letters, Vol.83, No.3-4, 201-207, 2002
n-butane isomerization over SO4=/NiO/Al2O3/ZrO2 catalysts. Effect of the reaction pressure and metal loading
The effect of alumina and nickel in sulfated ZrO2 as a catalyst for n-butane isomerization was investigated. Samples were synthesized by supporting nickel sulfated zirconia on boehmite and then calcining the material. The crystalline structure of ZrO2 was studied by X-ray powder diffraction and refined by the Rietveld method. Surface areas were determined by N-2 adsorption and BET analysis, while the acid properties were studied by NH3 adsorption. The chemical reaction was carried out in a fixed-bed microreactor at 338 K under atmospheric (78 kPa) or 245 kPa total pressure. Results showed that either nickel or alumina improved the catalytic activity, but a synergic effect was observed when both components assisted. The catalytic activity was related to the relative content of tetragonal zirconia and acid site density. Alumina stabilized tetragonal zirconia increased the acid site density and presumably led to a better dispersion of nickel oxide. The catalytic activity could be related to both oxidation and acid sites produced by nickel. A bimolecular reaction mechanism helps explain the observed trends. The increase in the reaction rate would be explained by the increase in the rate of the initial step of dehydrogenation either caused by a better dispersion of nickel or higher operating pressure.
Keywords:sulfated zirconia;nickel-alumina-promoted sulfated zirconia;mixed oxides;n-butane isomerization;tetragonal and monoclinic zirconia