Efficient and Highly Selective CO2 Capture, Separation, and Chemical Conversion under Ambient Conditions by a Polar-Group-Appended Copper(II) Metal-Organic Framework

A polar sulfone-appended copper(II) metal-organic framework (MOF; 1) has been synthesized from the dual-ligand approach comprised of tetrakis(4-pyridyloxymethylene)methane and dibenzothiophene-5,5'-dioxide-3,7-dicarboxylic acid under solvothermal conditions. This has been studied by different techniques that included single-crystal X-ray diffractometry, based on which the presence of Lewis acidic open-metal sites as well as polar sulfone groups aligned on the pore walls is identified. MOF 1 displays a high uptake of CO2 over N-2 and CH4 with an excellent selectivity (S = 883) for CO2/N-2 (15:85) at 298 K under flue gas combustion conditions. Additionally, the presence of Lewis acidic metal centers facilitates an efficient size-selective catalytic performance at ambient conditions for the conversion of CO2 into industrially valuable cyclic carbonates. The experimental investigations for this functional solvent-free heterogeneous catalyst are also found to be in good correlation with the computational studies provided by configurational bias Monte Carlo simulation for both CO2 capture and its conversion.

Automated summary

A polar sulfone-appended copper(II) metal-organic framework with Lewis acidic metal centers demonstrates high efficiency and selectivity in CO2 absorption, as well as excellent catalytic performance for converting CO2 into cyclic carbonates. Experimental investigations align closely with computational studies for both CO2 capture and conversion.