An unprecedented water stable acylamide-functionalized metal–organic framework for highly efficient CH4/CO2 gas storage/separation and acid–base cooperative catalytic activity†,Inorganic Chemistry Frontiers

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An unprecedented water stable acylamide-functionalized metal–organic framework for highly efficient CH4/CO2 gas storage/separation and acid–base cooperative catalytic activity†
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2018-08-02 00:00:00 , DOI: 10.1039/c8qi00662h
Baishu Zheng _{1,

2,

3,

4,

5} , Xin Luo _{1,

2,

3,

4,

5} , Zhaoxu Wang _{1,

2,

3,

4,

5} , Shaowei Zhang _{1,

2,

3,

4,

5} , Ruirui Yun _{6,

7,

8,

9} , Lu Huang _{1,

2,

3,

4,

5} , Wenjiang Zeng _{1,

2,

3,

4,

5} , Wenlong Liu _{9,

10,

11,

12}

Affiliation

The high porosity, excellent water stability and optimized supramolecular host–guest interactions of MOFs are the three key factors for their potential practical applications in many important areas including gas storage/separation, catalysis and so on. In this study, we designed and constructed a highly porous (3, 36)-connected txt-type acylamide-functionalized metal–organic framework (HNUST-8) from a pyridine-based acylamide-linking diisophthalate and dicopper(II)-paddlewheel clusters. Interestingly, HNUST-8 possesses an exceptionally water-stable framework with a high BET surface area of about 2800 m² g⁻¹. At 298 K, HNUST-8 exhibits a high excess CO₂ uptake of 19.7 mmol g⁻¹ at 40 bar, an excellent total CH₄ storage capacity of 223 cm³(STP) cm⁻³ with a large working capacity of 178 cm³(STP) cm⁻³ at 80 bar, as well as highly efficient CO₂/CH₄ and CO₂/N₂ separation under dynamic conditions at 1 bar. Moreover, with the Lewis acidic open copper(II) sites and Lewis basic acylamide groups integrated into the framework, HNUST-8 demonstrates efficient catalytic activity as an acid–base cooperative catalyst in a tandem one-pot deacetalization–Knoevenagel condensation reaction.

中文翻译：

前所未有的水稳定性酰基酰胺官能化的金属有机框架，可实现高效的CH ₄ / CO ₂气体存储/分离和酸碱协同催化活性†

MOF的高孔隙率，出色的水稳定性和优化的超分子主客体相互作用是它们在许多重要领域（包括储气/分离，催化等）中潜在实际应用的三个关键因素。在这项研究中，我们设计并构建了由吡啶基的酰胺基连接的二间苯二酸酯和dicopper（II）-叶轮簇组成的高度多孔（3，36 ）连接的txt型酰基酰胺官能化的金属有机骨架（HNUST-8）。。有趣的是，HNUST-8具有异常稳定的水构架，具有约2800 m ² g ^-1的高BET表面积。在298 K时，HNUST-8表现出19.7 mmol g ^-1的高过量CO ₂吸收在40 bar下，出色的CH ₄总存储容量为223 cm ³（STP）cm ^-3，在80 bar下具有178 cm ³（STP）cm ^-3的大工作容量，以及高效的CO ₂ / CH ₄在1 bar的动态条件下进行CO ₂ / N ₂分离。此外，通过将路易斯酸性开放铜（II）位点和路易斯碱性酰胺基团整合到框架中，HNUST-8在串联一锅脱缩醛-Knoevenagel缩合反应中表现出作为酸碱协作催化剂的有效催化活性。

更新日期：2018-08-02

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