Scalable Main Group Mechanocatalytic CO2 Valorisation to Cyclocarbonate Species

21 January 2025, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

Over the past two decades, main group elements have gained attention as promising substitutes for precious metals in catalytic processes. Additionally, mechanochemistry is emerging as a field with the potential to promote catalytic reactions under mild conditions. Herein, we report a scalable, main-group mechanocatalytic synthesis of cyclic carbonates from both solid and liquid epoxides, using CO₂ as a renewable feedstock under mild conditions with a gallium aminotrisphenolate catalyst. Unlike solution-based methods, which generally require high temperatures and/or high CO₂ pressures, this mechanocatalytic process operates at just 1 bar and room temperature. The developed mechanochemical method affords the targetted compounds in high yields, while also enabling efficient transformation of multi-terminal epoxides and avoiding the conversion losses typically observed in solution. Furthermore, this scalable method outperforms solution-based approaches across all green metrics, setting a new benchmark for environmentally friendly synthesis.

Keywords

Mechanochemistry
mechanocatalysis
CO2 valorisation
green metrics

Supplementary materials

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General information Experimental procedures Description of general procedure for the Gallium complex in pictures Description of general procedure for the cyclic carbonates in pictures Description of upscaling procedure 1H and 13C{1H} NMR data Green metrics calculation Table S2 with the green metrics of solution and mechanochemical GaLMe catalysis. Table S3 with the E-factors from selected solution-based catalysts. References
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