Leibniz-Institute for Catalysis at the University of Rostock, Albert-Einstein-Strasse 29a, 18059, Rostock, Germany.
Leibniz-Institute for Plasma Science and Technology (INP), Felix-Hausdorff-Strasse 2, 17489, Greifswald, Germany.
ChemSusChem. 2020 Apr 7;13(7):1825-1833. doi: 10.1002/cssc.201903384. Epub 2020 Mar 17.
The first plasma-assisted immobilization of an organocatalyst, namely a bifunctional phosphonium salt in an amorphous hydrogenated carbon coating, is reported. This method makes the requirement for prefunctionalized supports redundant. The immobilized catalyst was characterized by solid-state C and P NMR spectroscopy, SEM, and energy-dispersive X-ray spectroscopy. The immobilized catalyst (1 mol %) was employed in the synthesis of cyclic carbonates from epoxides and CO . Notably, the efficiency of the plasma-treated catalyst on SiO was higher than those of the SiO support impregnated with the catalyst and even the homogeneous counterpart. After optimization of the reaction conditions, 13 terminal and four internal epoxides were converted with CO to the respective cyclic carbonates in yields of up to 99 %. Furthermore, the possibility to recycle the immobilized catalyst was evaluated. Even though the catalyst could be reused, the yields gradually decreased from the third run. However, this is the first example of the recycling of a plasma-immobilized catalyst, which opens new possibilities in the recovery and reuse of catalysts.
首次报道了一种有机催化剂（双功能鏻盐）在非晶氢化碳涂层中的等离子体辅助固定化。该方法使得对预官能化载体的需求变得多余。通过固态 C 和 P NMR 光谱、SEM 和能量色散 X 射线光谱对固定化催化剂进行了表征。固定化催化剂（1 mol%）用于从环氧化物和 CO 合成环状碳酸酯。值得注意的是，等离子体处理的 SiO 上催化剂的效率高于催化剂浸渍的 SiO 载体，甚至高于均相催化剂。在优化反应条件后，13 个末端和 4 个内部环氧化物与 CO 反应生成相应的环状碳酸酯，产率高达 99%。此外，还评估了固定化催化剂的回收可能性。尽管催化剂可以重复使用，但从第三次运行开始，产率逐渐下降。然而，这是首例等离子体固定化催化剂的回收利用，为催化剂的回收和再利用开辟了新的可能性。
