Highly efficient CO2 capture and conversion of a microporous acylamide functionalized rht-type metal–organic framework,Inorganic Chemistry Frontiers

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Highly efficient CO2 capture and conversion of a microporous acylamide functionalized rht-type metal–organic framework
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2020-03-28 , DOI: 10.1039/d0qi00231c
Junxiong Liao _{1,

2,

3,

4,

5} , Wenjiang Zeng _{1,

2,

3,

4,

5} , Baishu Zheng _{1,

2,

3,

4,

5} , Xiyang Cao _{1,

2,

3,

4,

5} , Zhaoxu Wang _{1,

2,

3,

4,

5} , Guanyu Wang _{1,

2,

3,

4,

5} , Qingyuan Yang _{6,

7,

8,

9}

Affiliation

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 C₂-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 m² 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/N₂ 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.

中文翻译：

高效CO2捕获和微孔酰基酰胺官能化的rht型金属-有机骨架的转化

具有优异的骨架稳定性和优化的超分子主体-客体相互作用的高孔隙度MOF的设计与合成是获得用于目标应用（例如气体存储，分离，催化等）的高性能MOF材料的有效策略。在这里，我们从双铜（II）-桨轮簇和新型的C ₂对称的酰胺键连接的六羧酸酯中设计并构建了微孔（3，24）连接的rh型酰基酰胺官能化的MOF（HNUST-9）。有趣的是，高强度的强CO ₂结合位点包括开放的铜（II）位点和整合在骨架中的酰基酰胺基团，尽管显示出适度的孔隙度（BET表面积为2429 m ² g ^-1），但活化的HNUST-9却表现出异常高的CO ₂吸收能力（在25时为21.8 mmol g ^-1） bar和273 K），以及在1 bar和室温下的动态条件下从CO ₂ / CH ₄和CO ₂ / N ₂二元气体混合物中有效分离CO _2的能力。此外，HNUST-9表现出对CO _2的有效催化活性在温和，无溶剂的条件下，在四丁基溴化铵作为助催化剂的存在下，与各种环氧化物进行环加成反应。

更新日期：2020-03-28

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