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Amine-functionalized frameworks as highly actives catalysts for chemical fixation of CO2 under solvent and co-catalyst free conditions
Journal of CO2 Utilization ( IF 7.7 ) Pub Date : 2020-07-14 , DOI: 10.1016/j.jcou.2020.101253
Mahdie Saghian , Saeed Dehghanpour , Massoomeh Sharbatdaran

Herein, we report the adoption of adjustable composition nitrogen-rich units via introduction of diverse amine groups to an unsaturated metal organic framework, MIL-100(Cr), and the application of the products obtained as novel catalysts in the aspect of CO2 cycloaddition reactions to afford cyclic carbonates in the absence of co-catalyst and solvent under mild conditions (60 °C, 1 MPa). Incorporation of amine groups to the frameworks leads to substantial increment in the catalytic performance of the structures. The concomitant presence of acidic and basic sites in the structure causes great conversion and selectivity in cycloaddition reactions even for large and bulky epoxides. The comparison of various groups of amines (2-aminopyridine, 1,2-phenylene diamine, 3-aminopyridine and ethylene diamine) incorporated on the surface with different orientations demonstrates the effect of the orientation type in catalytic activity. CO2 gas sorption measurement helps to better understand the process of catalytic activity. The pristine MOF is unable to progress the reaction without addition of co-catalyst.



中文翻译:

胺官能化骨架作为高活性催化剂,可在无溶剂和无助催化剂的条件下化学固定CO 2

本文中,我们报道了通过将各种胺基引入不饱和金属有机骨架MIL-100(Cr)中来采用可调组成的富氮单元,并将所得产物作为新型催化剂应用于CO 2方面在温和条件下(60°C,1 MPa)在不存在助催化剂和溶剂的条件下进行环加成反应,得到环状碳酸酯。胺基团结合到骨架上导致结构催化性能的显着提高。结构中酸性位点和碱性位点的同时存在,即使对于大而笨重的环氧化物,也能在环加成反应中实现很高的转化率和选择性。比较以不同取向掺入到表面上的各组胺(2-氨基吡啶,1,2-亚苯基二胺,3-氨基吡啶和乙二胺)证明了取向类型对催化活性的影响。一氧化碳2气体吸附测量有助于更好地了解催化活性的过程。没有添加助催化剂,原始的MOF无法进行反应。

更新日期:2020-07-14
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