Abstract Novel, efficient and multifunctional binary systems consisting of Fe-bisiminopyridine complexes and additives are presented as effective catalysts for the synthesis of cyclic carbonates from epoxides and carbon dioxide. Due to the synergistic effects arising from the presence of a hydrogen bond donor and a carbon dioxide activator in well-designed heteroleptic ligands, the catalysts exhibited excellent capabilities and selectivities in carbon dioxide utilization at 50 °C and 5 bar pressure under solvent-free conditions. The control experiments and DFT calculations proposed the cooperative mechanism with functional groups combined. The reaction scope was successfully expanded to the synthesis of oxazolidinones with N-alkyl substituted aziridines.

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