A biopolymer mediated efficient synthesis of cyclic carbonates from epoxides and carbon dioxide
A biopolymer mediated efficient synthesis of cyclic carbonates from epoxides and carbon dioxide
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DOI：
10.1039/c2gc35942a
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发表时间：
2012-10
期刊：
影响因子：
9.8
通讯作者：
K. Roshan;George Mathai;Juntae Kim;J. Tharun;Gyung-Ah Park;Dae-Won Park
中科院分区：
文献类型：
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作者：
K. Roshan;George Mathai;Juntae Kim;J. Tharun;Gyung-Ah Park;Dae-Won Park
本文研究了羧甲基纤维素（CMC）作为多种咪唑基离子液体催化剂的载体材料在CO2化学固定中的应用前景。固定化在羧甲基纤维素（CMIL）上的离子液体在温和无溶剂条件下，对二氧化碳与环氧丙烷（PO）的环加成反应生成碳酸丙烯（PC）具有较高的催化活性和选择性。基于B3LYP/6-31G （d,p）水平的密度泛函理论（DFT）计算，提出了一种新的途径，其中CMC上的羧基和羟基部分与卤化物离子协同作用，最终在环加成反应中结束。羧基甲基纤维素载体上的羧基实体通过强氢键稳定产物络合物，从而促进反应。催化剂体系具有良好的可重复使用性。
A promising application of carboxymethyl cellulose (CMC), which is a congener of the cellulose family, as a supporting material for a variety of imidazolium based ionic liquid catalysts in the chemical fixation of CO2 has been studied here. The ionic liquids immobilized on the carboxymethyl cellulose (CMIL) showed high catalytic activity and selectivity in the cycloaddition of carbon dioxide with propylene oxide (PO) resulting in propylene carbonate (PC) under mild and solvent free conditions. A new pathway was proposed based on the density functional theory (DFT) calculations performed at the B3LYP/6-31G (d,p) level, where the carboxyl and hydroxyl moieties on the CMC were found to act synergistically with the halide ions to eventuate in the cycloaddition reaction. The carboxyl group entities on the carboxymethyl cellulose support supposedly stabilize the product complex via strong hydrogen bonds, thereby promoting the reaction. The catalyst system also displayed good reusability.