Loading...
3 results
Search Results
Now showing 1 - 3 of 3
- Elucidation of the zeolite role on the hydrogenating activity of Pt-catalystsPublication . Mendes, Pedro; Gregório, André F. C.; Daudin, Antoine; Bouchy, Christophe; Silva, João; Ribeiro, M FilipaToluene hydrogenation was studied over model catalysts with a fixed hydrogenating function (Pt/Al2O3) mechanically mixed with either HUSY or HBEA zeolites. Such mechanical mixtures showed improved platinum turnover frequencies compared to single Pt/Al2O3. Comparing to Pt-impregnated zeolite catalysts, the mechanical mixtures have lower activities per site showing that the contribution of acid sites decreases (and so the hydrogenating activity) with increased distance between Pt clusters and acid sites. Therefore, toluene hydrogenation can be used as a powerful tool to evaluate Pt-acid site intimacy in bifunctional catalysts.
- A systematic study on mixtures of Pt/zeolite as hydroisomerization catalystsPublication . Mendes, Pedro; Marques Mota, Filipe; Silva, João; Ribeiro, M Filipa; Daudin, Antoine; Bouchy, ChristopheMixtures of bifunctional catalysts were studied in the hydroisomerization of n-hexadecane. The study focused on the impact of the properties of individual catalysts on the hybrid catalysts' performance. On the one hand, a Pt/HUSY catalyst was mixed with a series of Pt/zeolites with different topologies and acidities, all of the catalysts being individually well-balanced. Despite the diversity of Pt/zeolite catalysts in terms of both activity and isomerization selectivity, the performances of the hybrid catalysts corresponded to the average of individual components. Cooperative effects are proposed to be caused by a great difference in the relative activity of the Pt/zeolite catalysts rather than in selectivity. On the other hand, mixtures of large-pore Pt/HUSY and Pt/HBEA catalysts with different Pt loadings were tested. The performance of the resulting hybrid catalysts was observed to be a function of global metal-acid balance. Mixtures of poorly-balanced and well-balanced catalysts can be at the origin of cooperative effects, as demonstrated experimentally by an improved C-16 isomer yield. The use of a dual-function kinetic model to simulate the performance of the hybrid catalysts corroborated these interpretations. This comprehensive work is expected to serve as a guideline for uncovering hybrid catalytic systems with industrial applications such as in the hydroisomerization of long chain n-paraffins.
- From powder to extrudate zeolite-based bifunctional hydroisomerization catalysts: on preserving zeolite integrity and optimizing Pt locationPublication . Mendes, Pedro; Silva, João; Ribeiro, M Filipa; Daudin, Antoine; Bouchy, ChristopheThe development of zeolite-based hydroisomerization catalysts in the powder form is widely spread in scientific literature but shaped bodies are the ones being employed in industry. This work aims at bridging that gap. The shaping procedure for HUSY zeolite in presence of an alumina binder disclosed herein achieved a full conservation of zeolite properties, e.g. porosity and Brønsted acidity. When Pt was located inside the zeolite and an homogeneous Pt distribution along the extrudate was ensured, shaped Pt-containing catalysts had similar hydroisomerization performances to those of powder Pt/zeolite in terms of turnover frequency per Brønsted acid site and maximal feed isomers yield. Conversely, non-uniform distribution of Pt along the extrudates diameter (millimetric scale) was observed to reduce the feed isomers yield. This was tentatively explained by the lower local metal to acid sites ratio in the core of the extrudates. Optimal performance of shaped bifunctional catalysts requires, hence, an adequate metal to acid sites ratio throughout the whole catalyst (i.e. at millimetric and nanometric scale), even if full intimacy between catalytic functions is ensured at the nanoscale by the selective deposition of Pt inside the zeolite.