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Integration of multifunctionalities on ionic liquid-anchored MIL-101(Cr): A robust and efficient heterogeneous catalyst for conversion of CO2 into cyclic carbonates
Microporous and Mesoporous Materials ( IF 5.2 ) Pub Date : 2020-11-10 , DOI: 10.1016/j.micromeso.2020.110750
Moliang Zou , Weili Dai , Pei Mao , Bing Li , Jie Mao , Shuqu Zhang , Lixia Yang , Shenglian Luo , Xubiao Luo , Jianping Zou

The rational integration of multiple functional components into a suitable matrix material is a promising strategy for constructing efficient catalysts for specific applications. Herein, a novel Zn-containing imidazolium bromide was facilely anchored onto MIL-101(Cr) (MIL-101(Cr)-(AIm)2ZnBr2) via a coordination bond between the amino group in ionic liquid (IL) moiety and unsaturated Cr3+ center in MOF framework, which catalyzed the efficient synthesis of cyclic carbonates through the cycloaddition of CO2 and epoxides. The as-prepared MIL-101(Cr)-(AIm)2ZnBr2 groups the essential factors that facilitate the superb cycloaddition efficiency, involving: (1) Cr (III) and Zn (II) working as Lewis acid sites for polarizing epoxide; (2) amino groups and ternary N species as Lewis basic sites for activating CO2; (3) Br anion as nucleophile to accelerate the opening of epoxy ring. Combining the high surface area (1146 m2/g) and numerous open pores, a high up to 97.3% of propylene carbonate yield and 100% of selectivity are achieved. Additionally, benefited from its good chemical stability, the catalyst maintains its high activity even after five successive runs. This work proposes a new strategy for constructing multifunctional catalyst for CO2 conversion by highlighting the synergistic effect enabled by one host.



中文翻译:

离子液体锚定的MIL-101(Cr)上的多功能集成:一种强大而有效的非均相催化剂,用于将CO 2转化为环状碳酸酯

将多种功能组分合理地整合到合适的基质材料中,是构建针对特定应用的高效催化剂的有前途的策略。在此,通过离子液体(IL)部分中的氨基与离子液体(IL)部分之间的配位键,将一种新型的含锌的溴化咪唑鎓轻松固定在MIL-101(Cr)(MIL-101(Cr)-(AIm)2 ZnBr 2)上。MOF骨架中的不饱和Cr 3+中心,通过CO 2和环氧化物的环加成反应催化了环状碳酸酯的有效合成。制备的MIL-101(Cr)-(AIm)2 ZnBr 2归纳了促进极好的环加成效率的基本因素,包括:(1)Cr(III)和Zn(II)作为路易斯酸位用于环氧化物极化;(2)氨基和三元氮作为激活CO 2的路易斯碱性位点;(3)溴-阴离子作为亲核试剂,以加速环氧环的开口。结合高表面积(1146 m 2 / g)和大量开孔,可实现高达97.3%的碳酸亚丙酯高收率和100%的选择性。此外,得益于其良好的化学稳定性,即使连续运行五次,该催化剂也能保持其高活性。这项工作提出了一种构建CO 2多功能催化剂的新策略。 通过突出一台主机启用的协同效应来实现转换。

更新日期:2020-11-12
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