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A room temperature synthesizable zeolitic imidazolium framework catalyst for the solvent-free synthesis of cyclic carbonates
Journal of CO2 Utilization ( IF 7.7 ) Pub Date : 2018-03-12 , DOI: 10.1016/j.jcou.2018.03.006
Robin Babu , Seol-Hee Kim , Jintu Francis Kurisingal , Hyeon-Jun Kim , Gak-Gyu Choi , Dae-Won Park

A zinc-based zeolitic imidazolium framework ZIF-71 was synthesized at room temperature and its structural and physical properties were exploited for the CO2-epoxide cycloaddition reactions. ZIF-71 is found to catalyze the synthesis of cyclic carbonates under both high (120 °C, co-catalyst free) and low temperature (room temperature, with co-catalyst) conditions with >99% selectivity. The reaction conditions, turnover frequency (TOF), selectivity, reusability and non-leaching properties of ZIF-71 was compared with that of the earlier reported Zn based ZIFs in this area of CO2 transformation and the results showed that the ZIF-71 reporting here stays along or a step ahead of the previously reported ZIFs. More than 99% selectivity to the final five-membered products was achieved by using ZIF-71 throughout the reactions; thereby the essential criterion of 100% atom economy is well maintained. With its permanent porosity and low leaching, the ZIF-71 catalyst is reusable for more than five times. Finally, a reaction mechanism for the catalytic activity of ZIF-71 was also proposed based on the previous density functional theory (DFT) studies.



中文翻译:

一种室温可合成的沸石咪唑骨架催化剂,用于无溶剂合成环状碳酸酯

在室温下合成了锌基沸石咪唑鎓骨架ZIF-71,并利用其结构和物理性质进行了CO 2-环氧化物的环加成反应。发现ZIF-71在高温(120°C,无助催化剂)和低温(室温,有助催化剂)条件下均以大于99%的选择性催化合成环状碳酸酯。将ZIF-71的反应条件,周转频率(TOF),选择性,可重复使用性和非浸出特性与该区域CO 2领域中较早报道的锌基ZIFs进行了比较。转换和结果表明,此处报告的ZIF-71沿用先前报告的ZIF或与之较前。通过在整个反应过程中使用ZIF-71,最终五元产物的选择性达到了99%以上;从而很好地保持了100%原子经济的基本标准。ZIF-71催化剂具有永久孔隙率和低浸出率,可重复使用超过五次。最后,基于先前的密度泛函理论(DFT)研究,还提出了ZIF-71催化活性的反应机理。

更新日期:2018-03-12
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