期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 8, 期 35, 页码 13185-13194出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.0c01736
关键词
Rare-earth metal complexes; Carbon dioxide; Cyclic carbonates; Kinetic study; Ambient conditions; Catalyst recycling
资金
- National Natural Science Foundation of China [21871198, 21674070]
- Major Research Project of the Natural Science of the Jiangsu Higher Education Institutions [19KJA360005]
- Project of Scientific and Technologic Infrastructure of Suzhou [SZS201708]
- Open Research Fund of State Key Laboratory of Rare Earth Resource Utilization (CIAC)
- PAPD
A series of rare-earth (RE) metal complexes (Y, Sm, Nd, and La) stabilized by polydentate N-methylethylenediamine-bridged tris(phenolato) ligands was synthesized and characterized. Lanthanum complexes showed good activity in catalyzing the cycloaddition reaction of terminal epoxides with CO2 under ambient conditions (i.e., room temperature, 1 bar CO2), giving rise to cyclic carbonates in 49-99% yields. More importantly, generally challenging internal epoxides were also transformed into cyclic carbonates in 70-99% yields in the presence of 1 bar CO2 at 60 degrees C. This is the first RE-based catalyst for efficient cycloaddition of CO2 and epoxides under ambient conditions and is among the most active catalysts for this important transformation. The lanthanum complex was also recycled six times. Kinetic study of the cycloaddition of cyclohexene oxide and CO2 was conducted, and the kinetic equation was determined as follows: rate = k[epoxide](1)[CO2](0)[cat.](1.26)[TBAI](0.4). The Gibbs activation energy (333 K) was determined to be 29.8 kcal/mol.
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