Jiang Yichen, Li Dazhi, Zhao Yifei, Sun Jianmin
State Key Laboratory of Urban Water Resource and Environment, MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150080, China.
State Key Laboratory of Urban Water Resource and Environment, MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150080, China.
J Colloid Interface Sci. 2022 Jul 15;618:22-33. doi: 10.1016/j.jcis.2022.03.038. Epub 2022 Mar 10.
Hydrogen bond donor functionalized poly(ionic liquids) were incorporated into MIL-101 framework for synthesis of composites PIL-R@MIL-101 (R = COOH, OH, NH). The effect of different hydrogen bond donors on CO-epoxide cycloaddition reaction was discussed through XPS, NH-TPD characterizations. Thereinto, PIL-COOH@MIL-101 showed efficient catalytic performance in the cycloaddition reaction of CO and epichlorohydrin, 92.7% substrate conversion was obtained under 70 °C, 1.0 MPa, cocatalyst- and solvent-free conditions for 2.5 h. The improved activity was benefited from the synergistic effects of Lewis acidic Cr centers, carboxyl group, and nucleophilic Br, together with the high surface area (1178 m/g), and good CO affinity. In addition, PIL-COOH@MIL-101 also showed facile recovery method by easy centrifugation and good recycling stability. Considering the good CO affinity, excellent catalytic performance in CO cycloaddition reaction, better thermal and recycling stabilities, the facilely prepared functionalized poly(ionic liquid)@MIL-101 composite would exhibit promising application prospect in CO capture and conversion.
将氢键供体功能化的聚离子液体引入MIL-101骨架中,用于合成复合材料PIL-R@MIL-101(R = COOH、OH、NH)。通过XPS、NH-TPD表征探讨了不同氢键供体对CO-环氧加成反应的影响。其中,PIL-COOH@MIL-101在CO与环氧氯丙烷的环加成反应中表现出高效的催化性能,在70℃、1.0MPa、无共催化剂和无溶剂条件下反应2.5h,底物转化率可达92.7%。活性的提高得益于路易斯酸性Cr中心、羧基和亲核Br的协同作用,以及高比表面积(1178 m²/g)和良好的CO亲和力。此外,PIL-COOH@MIL-101还具有通过简单离心实现的简便回收方法和良好的循环稳定性。考虑到其良好的CO亲和力、在CO环加成反应中优异的催化性能、较好的热稳定性和循环稳定性,这种简便制备的功能化聚离子液体@MIL-101复合材料在CO捕获和转化方面将展现出广阔的应用前景。