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Niobium on BEA Dealuminated Zeolite for High Selectivity Dehydration Reactions of Ethanol and Xylose into Diethyl Ether and Furfural

In this work, we investigated the role of solid-state dealumination by (NH(4))(2)SiF(6) (25% Al removal and 13% Si insertion), the impregnation of niobium (10, 18, and 25 wt. %) on dealuminated *BEA (DB) zeolite and their catalytic properties in ethanol and xylose transformations. Among all the stud...

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Detalles Bibliográficos
Autores principales: Valadares, Deborah S., Clemente, Maria Clara H., de Freitas, Elon F., Martins, Gesley Alex V., Dias, José A., Dias, Sílvia C. L.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: MDPI 2020
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7407447/
https://www.ncbi.nlm.nih.gov/pubmed/32610528
http://dx.doi.org/10.3390/nano10071269
Descripción
Sumario:In this work, we investigated the role of solid-state dealumination by (NH(4))(2)SiF(6) (25% Al removal and 13% Si insertion), the impregnation of niobium (10, 18, and 25 wt. %) on dealuminated *BEA (DB) zeolite and their catalytic properties in ethanol and xylose transformations. Among all the studied catalysts, 18%Nb-DB showed increased mesoporosity and external areas. A leveling effect in the number and strength of the proposed two sites (Brønsted and Lewis) present in the catalyst (n(1) = 0.24 mmol g(−1), −ΔH(1) = 49 kJ mol(−1), and n(2) = 0.20 mmol g(−1), –ΔH(2) = 42 kJ mol(−1)) in the catalyst 18%Nb-DB, might be responsible for its good activity. This catalyst presented the highest selectivity for diethyl ether, DEE (97%) with 61% conversion after 50 ethanol pulses at 230 °C (turnover number, TON DEE = 1.15). These features allowed catalytically fruitful bonding of the ethanol molecules to the neighboring sites on the channels, facilitating bimolecular ether formation through a possible SN(2) mechanism. The same catalyst was active and selective for transformation of xylose at 180 °C, showing 64% conversion and 51% selectivity for furfural (TON Furfural = 24.7) using water as a green solvent.