Highly Efficient Co2 Capture And Conversion Of A Microporous Acylamide Functionalized Rht-Type Metal-Organic Framework

INORGANIC CHEMISTRY FRONTIERS(2020)

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摘要
The design and synthesis of highly porous MOFs with excellent framework stability and optimized supramolecular host-guest interactions is an effective strategy to obtain high-performance MOF materials for targeted applications such as gas storage, separation, catalysis and so on. Herein, we designed and constructed a microporous (3, 24)-connected rht-type acylamide functionalized MOF (HNUST-9) from dicopper(ii)-paddlewheel clusters and a novel C-2-symmetric acylamide-linking hexacarboxylate. Interestingly, with a high density of strong CO2 binding sites including open copper(ii) sites and acylamide groups integrated in the framework, although exhibiting moderate porosity (a BET surface area of 2429 m(2) g(-1)), the activated HNUST-9 shows an exceptionally high excess CO2 uptake capacity (21.8 mmol g(-1) at 25 bar and 273 K), and efficient CO2 separation ability from CO2/CH4 and CO2/N-2 binary gas mixtures under dynamic conditions at 1 bar and room temperature. Moreover, HNUST-9 demonstrates efficient catalytic activity for the CO2 cycloaddition with various epoxides in the presence of tetrabutylammonium bromide as the cocatalyst under mild, solvent-free conditions.
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