On the real catalytically active species for CO2 fixation into cyclic carbonates under near ambient conditions: Dissociation equilibrium of [BMIm][Fe(NO)2Cl2] dependant on reaction temperature
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Otros documentos de la autoría: Leu, Meike K.; Vicente, Isabel; Alves Fernandes, Jesum; de Pedro, manuel; Dupont, Jairton; Sans, Victor; Licence, Peter; Gual, Aitor; Cano, Israel
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Mostrar el registro completo del ítemcomunitat-uji-handle:10234/9
comunitat-uji-handle2:10234/160292
comunitat-uji-handle3:10234/160293
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Título
On the real catalytically active species for CO2 fixation into cyclic carbonates under near ambient conditions: Dissociation equilibrium of [BMIm][Fe(NO)2Cl2] dependant on reaction temperatureAutoría
Fecha de publicación
2019-05-15Editor
ElsevierISSN
0926-3373Cita bibliográfica
LEU, Meike K., et al. On the real catalytically active species for CO2 fixation into cyclic carbonates under near ambient conditions: Dissociation equilibrium of [BMIm][Fe (NO) 2Cl2] dependant on reaction temperature. Applied Catalysis B: Environmental, 2019, vol. 245, p. 240-250Tipo de documento
info:eu-repo/semantics/articleVersión de la editorial
https://www.sciencedirect.com/science/article/pii/S0926337318312153Versión
info:eu-repo/semantics/acceptedVersionPalabras clave / Materias
Resumen
An imidazolium based iron-containing ionic liquid [BMIm][Fe(NO)2Cl2] (BMIm = 1-n-butyl-3-methyl-imidazolium) has been synthesized for the first time and fully characterized employing a wide range of techniques. The ... [+]
An imidazolium based iron-containing ionic liquid [BMIm][Fe(NO)2Cl2] (BMIm = 1-n-butyl-3-methyl-imidazolium) has been synthesized for the first time and fully characterized employing a wide range of techniques. The iron-based containing ionic liquid was found to be an active catalyst for the cycloaddition of CO2 to epoxides, giving high conversions for various substrates under near ambient conditions. In addition, the catalytic system showed a good recycling performance for five consecutive reaction cycles. Key mechanistic studies demonstrated that a bifunctional catalytic system is generated in situ by the partial dissociation of the iron-based ionic liquid into [BMIm][Cl], which results in a very efficient catalyst without the need of any additive or co-catalyst. The metal center plays a role as Lewis acid and activate the epoxide group, and the chloride anion, as part of [BMIm][Cl] moiety, acts as nucleophile and leads to the ring opening through a nucleophilic attack on the less sterically-hindered Cβ. The process is favoured by an interaction via H-bonding between the substrate and the H–C2 of the imidazolium ring, as was demonstrated by additional experiments. Kinetic studies indicated that the process followed first-order kinetics with respect to epoxide concentration and proved the existence of a reversible coordination/de-coordination equilibrium in which the active species are generated from the [BMIm][Fe(NO)2Cl2] complex. [-]
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Applied Catalysis B: Environmental, 2019, vol. 245Proyecto de investigación
Engineering & Physical Sciences Research Council (EPSRC): EP/L015633/1; European Community through a Marie Sklodowska-Curie Individual Fellowships (IF-EF): 704710; Engineering & Physical Sciences Research Council (EPSRC)Derechos de acceso
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