Wen Qin, Yuan Xuexin, Zhou Qiqi, Yang Hai-Jian, Jiang Qingqing, Hu Juncheng, Guo Cun-Yue
Key Laboratory of Catalysis and Energy Materials Chemistry of Education & Hubei Key Laboratory of Catalysis and Materials Science, College of Chemistry and Materials Science, South-Central Minzu University, Wuhan 430074, China.
School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China.
Materials (Basel). 2023 Feb 16;16(4):1646. doi: 10.3390/ma16041646.
A series of bifunctional Schiff base metal catalysts (Zn-NPClR, Zn-NPXH, and M-NPClH) with two quaternary ammonium groups were prepared for carbon dioxide (CO) and epoxide coupling reactions. The effects of the reaction variables on the catalytic activity were systematically investigated, and the optimal reaction conditions (120 °C, 1 MPa CO, 3 h) were screened. The performances of different metal-centered catalysts were evaluated, and Co-NPClH showed excellent activity. This kind of bifunctional catalyst has a wide range of substrate applicability, excellent stability, and can be reused for more than five runs. A relatively high TOF could reach up to 1416 h with Zn-NPClH as catalyst by adjusting reaction factors. In addition, the kinetic study of the coupling reaction catalyzed by three catalysts (Zn, Co, and Ni) was carried out to obtain the activation energy () for the formation of cyclic carbonates. Finally, a possible mechanism for this cyclization reaction was proposed.
制备了一系列带有两个季铵基团的双功能席夫碱金属催化剂（Zn-NPClR、Zn-NPXH和M-NPClH）用于二氧化碳（CO₂）与环氧化物的偶联反应。系统研究了反应变量对催化活性的影响，并筛选出最佳反应条件（120℃、1MPa CO₂、3h）。评估了不同金属中心催化剂的性能，Co-NPClH表现出优异的活性。这种双功能催化剂具有广泛的底物适用性、优异的稳定性，并且可以重复使用超过五次。通过调整反应因素，以Zn-NPClH为催化剂时，相对较高的TOF可达1416 h⁻¹。此外，对三种催化剂（Zn、Co和Ni）催化的偶联反应进行了动力学研究，以获得形成环状碳酸酯的活化能（Ea）。最后，提出了该环化反应的可能机理。
