Integrated activation and conversion of CO2 and propargylamine by a robust multi-active site copper catalyst

The conversion of carbon dioxide (CO 2 ) and propargylamines to 2-oxazolidinones is an essential reaction in industry, but efficiently activating both feedstocks remains a huge challenge for majority of catalysts. Herein, we developed a long-term stable copper catalyst, co-coordinated with sugar acetates (acetylglucose, AcGlu) and 2-methyl-imidazolium (Im-Cu A ). This catalyst features multi-active site, enabling it to efficiently capture and activate CO 2 , activate propargylamines, and stabilize the catalyst species simultaneously. As expected, 2-oxazolidinone was synthesized by this cyclization reaction with an exciting turnover frequency of 880 h −1 , which is around 180 times higher than that of CuCl 2 . Moreover, the catalytic activity of Im-Cu A did not decrease even after 20 replicates, which is exceptionally rare for homogeneous catalysts. Density functional theory calculations indicate that the electron-donating AcGlu and 2-methyl-imidazolium units facilitate electrons transport from Im-Cu A to CO 2 . Moreover, the high electron density of AcGlu and 2-methyl-imidazolium groups is believed to play a crucial role in the long-term stability across various temperatures and excellent catalytic performance of Im-Cu A . This represents a significant advancement in the development of a highly stable copper catalyst with multi-active site that effectively activates all reaction substrates. This strategy could improve the development of metal catalysts with sustained superior performance for CO 2 conversion.