期刊
CATALYSIS IN INDUSTRY
卷 5, 期 1, 页码 61-73出版社
MAIK NAUKA-INTERPERIODICA
DOI: 10.1134/S2070050413010030
关键词
paraffin dehydrogenation; MgAl2O4 support; mechanochemical synthesis; PtSnIn and PtSnGa supported catalysts; characterization of supported catalysts
资金
- Secretaria de Ciencia y Tecnica - Universidad Nacional del Litoral (CAI+D Program)
- ANPCYT
The catalytic performance in n-butane dehydrogenation of bimetallic PtSn, PtGa and PtIn, and trimetallic PtSnIn and PtSnGa catalysts (with low metal contents) supported on a MgAl2O4 prepared by a novel mechanochemical synthesis was evaluated both in flow and pulse equipment. The influence of the addition of different promoters (Sn, Ga and In) to Pt on the activity, selectivity and deactivation in the n-butane dehydrogenation reaction was studied. Stability experiments through successive reaction-regeneration cycles were carried out for selected catalysts. In order to correlate the properties of the metallic phase of the catalysts with the catalytic behavior, several characterization techniques were used, such as test reactions of the metallic phase (cyclohexane dehydrogenation and cyclopentane hydrogenolysis), TPR, XPS, H-2 chemisorption and TEM. Bimetallic PtSn catalyst has a better catalytic behavior than PtIn and PtGa ones. For PtSnM (M: In or Ga) catalysts, whereas Ga addition to the bimetallic catalyst does not practically modify the dehydrogenation performance, the addition of In produces an increase of the activity and the selectivity to butenes. Characterization results indicate the presence of geometric effects for the PtSn catalyst, and geometric and electronic effects for PtIn and PtGa ones. For trimetallic catalysts, the presence of a close contact between Pt, Sn and In or Ga in both trimetallic catalysts was found, mainly due to geometric effects like blocking and dilution of the active sites by the promoters. In stability experiments, the trimetallic PtSnIn/MgAl2O4 catalyst clearly displays the best catalytic performance along reaction-regeneration cycles, though PtSnGa and PtSn catalysts also showed a very good behavior through the successive cycles. The characterization of these catalysts after cycles shows that their metallic phases are slightly modified along the cycles.
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