Imidazolium-based titanosilicate nanospheres as active catalysts in carbon dioxide conversion: Towards a cascade reaction from alkenes to cyclic carbonates

Adrien Comès, Rémy Poncelet, Paolo P. Pescarmona, Carmela Aprile

Résultats de recherche: Contribution à un journal/une revueArticleRevue par des pairs


Porous silica-based nanospheres bearing titanium centres as single site were successfully synthesized employing a time- and energy-efficient procedure. The influence of the post-synthesis treatment on the insertion of Ti was investigated via DR UV-Vis and XPS spectroscopy and the titanium content was quantified through ICP-OES analysis. The textural and structural properties of the different solids were evaluated via XRD, TEM and N2 physisorption. The resulting materials were thereafter covalently functionalized with imidazolium chloride, followed by characterization via 29Si and 13C solid-state NMR, N2 physisorption and chemical combustion analysis. The bi-functional catalysts were tested in the challenging conversion of CO2 with cyclohexene oxide to the corresponding cyclic carbonate as well as with various other epoxides with excellent results. The insertion of Ti as single site played a key role substantially improving the activity of the solids. The most active bi-functional material was successfully recovered and reused through multiple cycle without loss of the catalytic activity. Moreover, the cyclohexene epoxidation reaction was tested as well employing the mono-functionalized Ti-based material. The catalytic mixture, composed by the mono-functional and bi-functional solids, was efficiently used to convert the cyclohexene into cyclohexene oxide and subsequently the cyclohexene oxide into the corresponding carbonate thus opening the prospect for a cascade reaction.

langue originaleAnglais
Numéro d'article101529
journalJournal of CO2 Utilization
Les DOIs
Etat de la publicationPublié - juin 2021

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