Different alkylamine molecules were post-synthetically tethered to the unsaturated CrIII centers in the metal–organic framework MIL-101. The resultant metal–organic frameworks show almost no N2 adsorption with significantly enhanced CO2 capture under ambient conditions as a result of the interaction between amine groups and CO2 molecules. Given the extraordinary stability, high CO2 uptake, ultrahigh CO2/N2 selectivity, and mild regeneration energy, MIL-101-diethylenetriamine holds exceptional promise for post-combustion CO2 capture and CO2/N2 separation.
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