Issue 12, 2022

Cycloaddition of di-substituted epoxides and CO2 under ambient conditions catalysed by rare-earth poly(phenolate) complexes

Abstract

A series of rare-earth (RE) metal complexes [RE = La (1, 5, 6), Nd (2), Sm (3), Y (4)] bearing polydentate N’-(2-aminoethyl)-N,N-dimethyl-1,2-ethylenediamine bridged-tris(phenolto) ligands were synthesized and characterized. The activity of complexes 1–6 for catalysing the cycloaddition reaction of CO2 and epoxides was studied, and the lanthanum complex 1 showed the highest activity. Under the conditions of 1 bar CO2 and 25 °C, lanthanum complex 1 catalysed the reaction of 18 mono-substituted epoxides, generating cyclic carbonates in 50–99% yields. More importantly, it also catalysed reactions of 6 di-substituted epoxides under ambient conditions (1 bar CO2 and 25 °C), and generated cyclic carbonates in 85–99% yields. This lanthanum complex is the first catalyst capable of converting di-substituted epoxides into internal cyclic carbonates under ambient conditions. Kinetic study was conducted to determine rate orders and Gibbs activation energy. A DFT study proved that poly(phenolto) ligands play vital roles in product dissociation.

Graphical abstract: Cycloaddition of di-substituted epoxides and CO2 under ambient conditions catalysed by rare-earth poly(phenolate) complexes

Supplementary files

Article information

Article type
Research Article
Submitted
19 Mar 2022
Accepted
22 Apr 2022
First published
28 Apr 2022

Inorg. Chem. Front., 2022,9, 2969-2979

Cycloaddition of di-substituted epoxides and CO2 under ambient conditions catalysed by rare-earth poly(phenolate) complexes

Y. Qing, T. Liu, B. Zhao, X. Bao, D. Yuan and Y. Yao, Inorg. Chem. Front., 2022, 9, 2969 DOI: 10.1039/D2QI00592A

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