Insight into the Varying Reactivity of Different Catalysts for CO2 Cycloaddition into Styrene Oxide: An Experimental and DFT Study

The cycloaddition of CO2 into epoxides to form cyclic carbonates is a highly sought-after reaction for its potential to both reduce and use CO2, which is a greenhouse gas. In this paper, we present experimental and theoretical studies and a mechanistic approach for three catalytic systems. First, as...

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Bibliographic Details
Published in:International journal of molecular sciences 2023-02, Vol.24 (3), p.2123
Main Authors: Sebaaly, Angelo Pio, Dias, Hugo, Christ, Lorraine, Merzoud, Lynda, Chermette, Henry, Hoffmann, Guillaume, Morell, Christophe
Format: Article
Language:English
Subjects:
Acids
Carbon dioxide
Carbonates
catalysis
Catalysts
Chemical Sciences
Chemists
Climate change
CO2 capture
Cycloaddition
DFT
Energy
Epoxides
Greenhouse gases
Hydrogen bonds
Imidazole
Lewis acid
Lewis base
mechanistic study
non-covalent interactions
Radiation
Reactivity
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Summary:The cycloaddition of CO2 into epoxides to form cyclic carbonates is a highly sought-after reaction for its potential to both reduce and use CO2, which is a greenhouse gas. In this paper, we present experimental and theoretical studies and a mechanistic approach for three catalytic systems. First, as Lewis base catalysts, imidazole and its derivatives, then as a Lewis acid catalyst, ZnI2 alone, and after that, the combined system of ZnI2 and imidazole. In the former, we aimed to discover the reasons for the varied reactivities of five Lewis base catalysts. Furthermore, we succeeded in reproducing the experimental results and trends using DFT. To add, we emphasized the importance of non-covalent interactions and their role in reactivity. In our case, the presence of a hydrogen bond was a key factor in decreasing the reactivity of some catalysts, thus leading to lower conversion rates. Finally, mechanistically understanding this 100% atom economy reaction can aid experimental chemists in designing better and more efficient catalytic systems.
ISSN:1422-0067
1661-6596
1422-0067
DOI:10.3390/ijms24032123