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Dialkylpyrazolium ionic liquids as novel catalyst for efficient fixation of CO2 with metal- and solvent-free
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2017-09-08 , DOI: 10.1016/j.apcata.2017.09.009
Yuan Ma , Ci Chen , Tengfei Wang , Jingshun Zhang , JiaJia Wu , Xiangdong Liu , Tiegang Ren , Li Wang , Jinglai Zhang

The efficient fixation of CO2 without co-catalyst and solvent under metal-free condition is still an urgent topic in sustainable chemistry. In this work, a series of dialkylpyrazolium ionic liquids are employed to promote the cycloaddition of CO2 and PO to produce PC. They would be easily synthesized by a simple one-pot reaction. The effect of alkyl chain length in cation and different anion is explored. Diethylpyrazolium iodide presents the excellent catalytic activity with the product yield of 96% and selectivity of 99% in a benign condition. Moreover, the catalyst could be reused for at least five times without significant loss of catalytic activity. An intensive structure-activity research testifies that the cycloaddition of CO2 with PO is activated by a synergistic effect from both cation and anion of ILs. To confirm it, the detailed mechanism is investigated by density functional theory associated with the non-covalent interactions and atoms in molecule analysis. Besides the electrostatic interaction between cation of ionic liquid and PO, the noncovalent interaction, especially for hydrogen bond, plays a vital role in promoting the reaction.



中文翻译:

二烷基吡唑鎓离子液体作为新型催化剂,可在无金属和无溶剂的情况下有效固定CO 2

在无金属条件下,没有助催化剂和溶剂的情况下如何有效地固定CO 2仍然是可持续化学领域的紧迫课题。在这项工作中,采用了一系列的二烷基吡唑鎓离子液体来促进CO 2和PO的环加成反应以生产PC。通过简单的一锅反应可以很容易地合成它们。探索了烷基链长度对阳离子和不同阴离子的影响。碘化二乙基吡唑鎓碘化物具有优良的催化活性,在良性条件下的产物收率为96%,选择性为99%。而且,该催化剂可以重复使用至少五次而不会显着降低催化活性。深入的结构活性研究证明,CO 2的环加成反应ILs的阳离子和阴离子的协同作用激活了PO。为了证实这一点,通过与非共价相互作用和分子分析中的原子有关的密度泛函理论研究了详细的机理。除了离子液体阳离子和PO之间的静电相互作用外,非共价相互作用(尤其是氢键)在促进反应中也起着至关重要的作用。

更新日期:2017-09-08
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