Covalent organic framework-supported Zn single atom catalyst for highly efficient N-formylation of amines with CO2 under mild conditions

Transformation of CO2 into value-added chemicals with efficient and recyclable catalyst is an effective way to reduce carbon emissions. It is valuable to develop an efficient catalyst that can promote the N-formylation reaction under mild conditions with a high activity and excellent recyclability. Single atom catalysts (SACs) possess ultimate atom utilization efficiency and outstanding catalytic performance. Herein, we synthesize Zn SACs (ZnTpPa) anchored on a COF (TpPa-1) using a facile solution method. Catalyzed by Zn-TpPa, CO2 and N-methylamine are transformed into N-methylformanilide under mild reaction conditions with a TOF of 17,155 h(-1), which is the highest among all reported recyclable Zn-based catalysts. Zn-TpPa can also catalyze N-formylation of many other amines with excellent yields. The higher reactivity was attributable to the well-dispersed Zn active sites on COF and outstanding adsorption of CO2 owing to high surface area of COF. Our research provides a facile method for constructing SACs as well as an effective pathway for CO2 transformation and environmental protection.

Automated summary

Developing efficient and recyclable catalysts for the transformation of CO2 into value-added chemicals is crucial for reducing carbon emissions. In this study, a highly efficient Zn single atom catalyst was synthesized, which can promote the N-formylation reactions of various amines under mild conditions with outstanding catalytic performance and high activity.