Highly Selective Carbon Dioxide Capture and Cooperative Catalysis of a Water‐Stable Acylamide‐Functionalized Metal–Organic Framework

Incorporation of specific functionalities within the framework offers a significant opportunity to produce high‐performance gas storage/separation and catalysis MOF materials. In this work, multifunctionalities, including hydrophobic methoxy groups, polar acylamide functionalities, and open copper(II) sites, have been successfully integrated into a twofold interpenetrated microporous MOF (HNUST‐6, HNUST represents Hunan University of Science and Technology). HNUST‐6 possesses permanent porosity, with a moderate BET surface area of 1093 m2 g–1 and high CO2 adsorption capacity (111 cm3 g–1 at 1 bar), with good selectivity for CO2 over CH4 (6.6) and N2 (30.3) at 273 K. Remarkably, this MOF material exhibits excellent water stability and its framework structure is retained after being immersed in boiling water. In addition, HNUST‐6 demonstrates efficient catalytic activity as a cooperative catalyst in a tandem one‐pot deacetalization Knoevenagel condensation reaction. A copper(II) microporous acylamide‐functionalized MOF, with a twofold interpenetrated and methoxy‐decorated framework, shows high and selective CO2 uptake under ambient temperature, with excellent water stability and cooperative catalytic activity, in a tandem deacetalization Knoevenagel condensation reaction.