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Catalytic transformation of CO2: from monomers to polymers
Alves, Margot; Grignard, Bruno; Boyaval, Amélie et al.
2016Belgian Polymer Group (BPG) Annual Meeting
 

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Keywords :
supercritical carbon dioxide
Abstract :
[en] Valorising CO2 as a renewable C1 feedstock for producing added value building blocks is the scope of many academic and industrial researches. Carbon dioxide is a thermodynamically and kinetically stable molecule that can be converted into five membered cyclic carbonates by coupling with epoxides using organometallic complexes or organocatalysts. To date, the identification and development of highly efficient (organo)catalysts under mild experimental conditions still remains challenging. In particular, the synthesis of six membered cyclic carbonates by the CO2/oxetane coupling using such organocatalysts has never been reported to our knowledge. In this context, we developed a new highly efficient bicomponent homogeneous organocatalyst composed of an ammonium salt as the catalyst and fluorinated single or double hydrogen bond donor activators (HBD). First, the efficiency of this new organocatalyst for the fast and selective CO2/epoxide coupling was investigated through detailed kinetic studies by IR spectroscopy under pressure and results were compared with the most efficient organocatalysts reported in the literature. This study was completed by molecular modeling in order to elucidate the reaction mechanism. DFT calculations showed that the hexafluoroisopropanol functionalities of HBDs strengthened the proton donor capability and allowed a better stabilization by hydrogen bonding of the intermediates and transition states. Finally, the use of this dual organocatalyst was extended to the coupling of CO2 with less reactive oxetanes to produce hydroxyl telechelic oligocarbonates.
Research center :
Center for Education and Research on Macromolecules (CERM)
Disciplines :
Chemistry
Materials science & engineering
Author, co-author :
Alves, Margot ;  University of Liège - ULiège > Department of Chemistry > Center for Education and Research on Macromolecules (CERM)
Grignard, Bruno ;  University of Liège - ULiège > Department of Chemistry > Center for Education and Research on Macromolecules (CERM)
Boyaval, Amélie ;  University of Liège - ULiège > Department of Chemistry > Center for Education and Research on Macromolecules (CERM)
Gennen, Sandro ;  University of Liège - ULiège > Department of Chemistry > Center for Education and Research on Macromolecules (CERM)
Méreau, Raphaël;  University of Bordeaux, Institute of Molecular Sciences, France
Tassaing, Thierry;  University of Bordeaux, Institute of Molecular Sciences, France
Detrembleur, Christophe ;  University of Liège - ULiège > Department of Chemistry > Center for Education and Research on Macromolecules (CERM)
De Winter, Julien;  University of Mons-Hainaut (UMH), Mass Spectrometry Research Group, Interdisciplinary Center of Mass Spectrometry (CISMa)
Gerbaux, Pascal;  University of Mons-Hainaut (UMH), Mass Spectrometry Research Group, Interdisciplinary Center of Mass Spectrometry (CISMa)
Jérôme, Christine  ;  University of Liège - ULiège > Department of Chemistry > Center for Education and Research on Macromolecules (CERM)
Language :
English
Title :
Catalytic transformation of CO2: from monomers to polymers
Publication date :
24 May 2016
Event name :
Belgian Polymer Group (BPG) Annual Meeting
Event place :
Hasselt, Belgium
Event date :
23/05/2016 - 25/05/2016
Funders :
The International Doctoral School IDS-Funmat
Commentary :
This oral communication was presented by Margot Alves
Available on ORBi :
since 31 May 2016

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