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Efficient Cycloaddition of CO2 and Aziridines Activated by a Quadruple-Interpenetrated Indium–Organic Framework as a Recyclable Catalyst
Inorganic Chemistry ( IF 4.6 ) Pub Date : 2021-09-30 , DOI: 10.1021/acs.inorgchem.1c02034
Xue-Rui Tian 1 , Ying Shi 1 , Sheng-Li Hou 1 , Yue Ma 1 , Bin Zhao 1
Affiliation  

On the basis of the global warming effect, it is of great significance to convert CO2 into the high value-added products oxazolidinones, but investigations on main-group-based metal–organic frameworks (MOFs) as heterogeneous catalysts still have not been reported so far. In this work, a quadruple-interpenetrated porous indium-based MOF, {[NH2(CH3)2][In(CPT)2]·3CH3CN·3DMA}n (1), is constructed from the organic ligand 3,5-bis(4′-carboxyphenyl)-1,2,4-triazole through solvothermal reactions, and N2 adsorption proves that the framework has a high Brunauer–Emmett–Teller surface areas with 2024 m2/g. The catalytic research on CO2 conversion reveals that compound 1 has high reactivity for the cycloaddition of CO2 with aziridines, and the product 3-ethyl-5-phenyloxazolidin-2-one can be obtained with a yield of 99% under mild conditions. In addition, 1 exhibits excellent activity for different kinds of substrates and can be reused at least five cycles without any significant deactivation, suggesting that 1 is a potential candidate for the chemical conversion of CO2 and aziridines. Mechanistic explorations indicate that the high efficiency of 1 is attributed to the indium center in the framework as a Lewis acid site, and the large porosity can enrich substrates. Importantly, 1 behaved as the first main-group MOF-based catalyst in the reported coupling reaction of CO2 with aziridines.

中文翻译:

四重互穿铟-有机骨架作为可回收催化剂活化的 CO2 和氮丙啶的有效环加成

基于全球变暖效应,将CO 2转化为高附加值产品恶唑烷酮具有重要意义,但基于主族的金属有机骨架(MOFs)作为多相催化剂的研究尚未见报道迄今为止。在这项工作中,由有机配体 3 构建了四重互穿多孔铟基 MOF,{[NH 2 (CH 3 ) 2 ][In(CPT) 2 ]·3CH 3 CN·3DMA} n ( 1 ) ,5-双(4'-羧基苯基)-1,2,4-三唑通过溶剂热反应和N 2吸附证明该框架具有2024 m 2的高Brunauer-Emmett-Teller表面积/G。CO 2转化催化研究表明,化合物1对CO 2与氮丙啶的环加成反应具有较高的反应活性,在温和条件下可以以99%的收率得到产物3-乙基-5-苯基恶唑烷-2-one。此外,1对不同种类的底物表现出优异的活性,并且可以重复使用至少五个循环而没有任何显着的失活,这表明1是 CO 2和氮丙啶化学转化的潜在候选者。机理探索表明,1归因于框架中的铟中心作为路易斯酸位点,大孔隙率可以丰富基材。重要的是,在报道的CO 2与氮丙啶的偶联反应中,1充当了第一个基于主族MOF 的催化剂。
更新日期:2021-10-18
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