Protic pyrazolium ionic liquids for efficient chemical fixation of CO2: design, synthesis, and catalysis
Protic pyrazolium ionic liquids for efficient chemical fixation of CO2: design, synthesis, and catalysis
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用于有效化学固定 CO2 的质子吡唑离子液体：设计、合成和催化
DOI：
10.1039/c7me00068e
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发表时间：
2018
影响因子：
3.6
通讯作者：
Jinglai Zhang
中科院分区：
文献类型：
--
作者：
Danning Zheng;Tengfei Wang;Xinrui Zhu;Ci Chen;Tiegang Ren;Li Wang;Jinglai Zhang
在良性条件下将二氧化碳转化为有机产品仍然具有挑战性。从可持续发展的角度来看，离子液体被视为高效且“绿色”的催化剂。然而，尽管吡唑鎓离子液体是咪唑鎓离子液体的结构异构体，但很少有人关注它们。对质子吡唑鎓离子液体的研究甚至更少。在这项工作中，合成了三种新的质子吡唑离子液体：HTMPzBr、HMM3PzBr 和 HMM5PzBr，以探索它们对二氧化碳和环氧丙烷偶联反应的催化活性。理论计算和实验表征均证实HTMPzBr和HMM5PzBr具有相似的催化活性，且高于HMM3PzBr。通过详细的理论分析阐明了反应中各种弱相互作用，特别是氢键的作用。 Double-IL理论模型预测的催化活性序列与实验结果完全一致。如果应用合适的理论模型，从分子水平设计离子液体是合理的，这将为进一步的实验研究提供一定的指导。
The conversion of carbon dioxide into organic products under benign conditions is still challenging. Ionic liquids are regarded as efficient and “green” catalysts from a sustainability view point. However, little attention has been focused on pyrazolium ILs although they are structural isomers of imidazolium ILs. Even fewer studies have been performed on protic pyrazolium ILs. In this work, three new protic pyrazolium ILs, HTMPzBr, HMM3PzBr, and HMM5PzBr, have been synthesized to explore their catalytic activity for the coupling reaction of carbon dioxide and propylene oxide. Both theoretical calculations and experimental characterization have verified that HTMPzBr and HMM5PzBr have similar catalytic activity, which is higher than that of HMM3PzBr. The role of various weak interactions, especially hydrogen bonds, in the reaction is elucidated by detailed theoretical analysis. The sequence of catalytic activity predicted by the Double-IL theoretical model is totally consistent with the experimental result. It is reasonable to design ionic liquids from a molecular level if a suitable theoretical model is applied, and this would provide some guidance for further experimental study.