Reordenamiento de Beckmann para la obtención del Monómero del Nylon 6 (Caprolactama) empleando como catalizadores materiales Mesoporosos Al-MCM-41
; Pratto, Jésica ; Arroqui, Pablo ; Herrero, Eduardo ; Casuscelli, Sandra Graciela
; Eimer, Griselda Alejandra 
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Fecha
09/2014
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Universidad Tecnológica Nacional
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Tecnología y Ciencia
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1666-6917
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Se sintetizaron catalizadores del tipo Al-MCM-41 modificando el contenido de Alumino. Los materiales se caracterizaron por: DRX, ICP-OES, RMN, FT-IR y adsorción de piridina acoplada a espectroscopia FT-IR. Se evaluaron cataliticamente los materiales sintetizados en la reacción de Reordenamiento de Beckmann para la obtención de ξ-Caprolactama a partir de ciclohexanona oxima. Se estudiaron las propiedades físico-químicas, el comportamiento ácido y el rendimiento catalítico. Se ha sugerido que los sitios activos para esta reacción son los silanoles nidos de carácter ácido de Bronsted débil asociados con la incorporación de Al en la red mesoporosa. Con la relación Si/Al=20 se logró la mayor cantidad de sitios ácidos (silanoles nidos) y 60% de rendimiento a ξ-Caprolactama con 100% de selectividad empleando condiciones de reacción suaves. Finalmente, con este catalizador, se variaron las condiciones de reacción obteniéndose conversiones del 94% y selectividad del 88% empleando 1-hexanol como solvente, T= 360°C y W/F= 40 gh/mol.
Al-MCM-41 catalysts were synthesized with different Aluminum content. The materials were characterized by XRD, ICP-OES, NMR, FT-IR absorption of pyridine and coupled to FT-IR spectroscopy.All the materials were catalytically evaluated in the Beckmann rearrangement reaction to obtain ξ-caprolactam from cyclohexanone oxime.The physicochemical properties, the catalytic yield and the acidity of the materials were studied. It has been suggested that the active sites for the Beckmann rearrangement are silanols nests (structural defects) of weak Bronsted acid character, closely associated with the incorporation of Al in the mesoporous network. In conclusion, with Si/Al = 20 it could be obtained the major proportion of acid sites and good performance to ξ-caprolactam (60%) with 100% selectivity. Finally, with this catalyst several reaction conditions were modified and the better results (conversions of 94% and selectivity of 88%) were obtained when 1-hexanol was used as a solvent, T= 360 °C and W/F = 40 gh/mol.
Al-MCM-41 catalysts were synthesized with different Aluminum content. The materials were characterized by XRD, ICP-OES, NMR, FT-IR absorption of pyridine and coupled to FT-IR spectroscopy.All the materials were catalytically evaluated in the Beckmann rearrangement reaction to obtain ξ-caprolactam from cyclohexanone oxime.The physicochemical properties, the catalytic yield and the acidity of the materials were studied. It has been suggested that the active sites for the Beckmann rearrangement are silanols nests (structural defects) of weak Bronsted acid character, closely associated with the incorporation of Al in the mesoporous network. In conclusion, with Si/Al = 20 it could be obtained the major proportion of acid sites and good performance to ξ-caprolactam (60%) with 100% selectivity. Finally, with this catalyst several reaction conditions were modified and the better results (conversions of 94% and selectivity of 88%) were obtained when 1-hexanol was used as a solvent, T= 360 °C and W/F = 40 gh/mol.
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