核壳型MOFs@离子液体复合材料的制备及其常压下催化CO2环加成反应性能探究

Construction of core-shell MOFs@ionic liquid materials and their performance for CO2 cycloaddition reaction under atmospheric pressure

  • 摘要: 通过双氨基功能化离子液体与对苯二甲醛原位共价组装得到柔性聚合物(DP),并采用后合成修饰法将DP包覆于金属有机框架材料MIL-101(Cr)表面,构筑了一种核-壳型复合材料(MIL-101@DP)用于催化CO2和环氧氯丙烷(ECH)环加成反应。MIL-101@DP保留了MIL-101(Cr)高比表面积和高孔隙率的优点,并兼具亲核位点Cl与Lewis酸性位点Cr3 + 。在Lewis酸碱位点协同作用下,MIL-101@DP可在常压、80 ℃、24 h且无助催化剂的条件下高效催化转化CO2和ECH反应(ECH转化率可达99%),且在循环使用四次后活性未出现明显下降。

     

    Abstract: A flexible polymer (DP) was prepared by in-situ covalent assembly of dual-amino-functionalized ionic liquids and terephthalaldehyde. A core-shell composite (MIL-101@DP) was constructed by coating DP on the surface of metal-organic frame material MIL-101 (Cr) by post-synthesis modification, and was applied to catalyze the cycloaddition reaction of CO2 and epichlorohydrin (ECH). MIL-101@DP retains the advantage of high specific surface area and high porosity of MIL-101 (Cr), and combines the nucleophilic site Cl and Lewis acidic site Cr3 + . Under the synergistic interaction of Lewis acid sites and Lewis base sites, MIL-101@DP could efficiently catalyze activity the conversion of CO2 and ECH reaction (ECH conversion rate can reach 99%) at atmospheric pressure, 80 ℃, 24 h and without cocatalyst. The activity did not decrease significantly after four cycles.

     

/

返回文章
返回