Reference : Heterogenization of a cyclocarbonation catalyst: optimization and kinetic study
Scientific journals : Article
Physical, chemical, mathematical & earth Sciences : Chemistry
Engineering, computing & technology : Materials science & engineering
http://hdl.handle.net/2268/229970
Heterogenization of a cyclocarbonation catalyst: optimization and kinetic study
English
Léonard, Géraldine L.-M. [Carmeuse Research and Technology SA, Louvain-la-Neuve, Belgium > > > >]
Belet, Artium [University of Liège (ULiège), Department of Chemical Engineering – Nanomaterials, Catalysis, Electrochemistry > > > >]
Grignard, Bruno [University of Liège (ULiège), Complex and Entangled Systems from Atoms to Materials (CESAM), Center for Education and Research on Macromolecules (CERM) > > > >]
Calberg, Cédric [University of Liège (ULiège), Department of Chemical Engineering – Nanomaterials, Catalysis, Electrochemistry > > > >]
Gilbert, Bernard [University of Liège (ULiège), Department of Chemistry, Laboratory of Raman Spectroscopy > > > >]
Jérôme, Christine mailto [University of Liège (ULiège), Complex and Entangled Systems from Atoms to Materials (CESAM), Center for Education and Research on Macromolecules (CERM) > > > >]
Heinrichs, Benoît mailto [University of Liège (ULiège), Department of Chemical Engineering – Nanomaterials, Catalysis, Electrochemistry > > > >]
In press
Catalysis Today
Yes (verified by ORBi)
International
0920-5861
1873-4308
[en] supercritical carbon dioxide
[en] Different types of heterogeneous catalysts designed for a cyclocarbonation reaction between an epoxidized source and CO2 under supercritical conditions have been synthesized. The process implied a quaternization step where a (haloalkyl)trimethoxysilane reacted with tributylamine leading to a tributyl(trimethoxysilylalkyl)ammonium halide, with iodine and bromine as halogens. Then, a grafting step onto commercial fumed silica through condensation reaction between the silane part and Si-OH surficial groups provided the immobilized catalyst. The efficiency of grafting has been validated by liquid 1H NMR, solid 29Si NMR and TG-DSC-MS analyzes. The benchmark cyclocarbonation reaction of polyethylene glycol diglycidylether at 80 °C and 100 bar during 4 h showed that the best immobilized catalyst was tributylpropylammonium iodide (IC3Q-EH5). It has also been shown that immobilization provided -surprisingly !- better conversions than the corresponding homogeneous catalyst’s: this phenomenon has been explained through an epoxide-ring-opening activating effect thanks to Si-OH surficial groups. Furthermore, kinetic studies performed by in situ Raman spectroscopy on IC3Q-EH5 showed that temperature had a strong influence on the yield of the reaction while CO2 pressure had only a small effect. Recycling of the catalyst has also been considered, but no precise conclusions could be conducted because of the high catalyst dispersion. Finally, the addition of a fluorinated alcohol co-catalyst allowed obtaining a similar yield but at 80 °C and 55 bar during only 2,5 h with the best candidate.
Complex and Entangled Systems from Atoms to Materials (CESAM) ; Center for Education and Research on Macromolecules (CERM)
The Walloon Region in the frame of the "CO2Green" project
Researchers
http://hdl.handle.net/2268/229970
10.1016/j.cattod.2018.11.060

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