Comès Adrien, Collard Xavier, Fusaro Luca, Atzori Luciano, Cutrufello M Giorgia, Aprile Carmela
Unit of Nanomaterial Chemistry (CNANO), University of Namur (UNAMUR), Department of Chemistry Rue de Bruxelles 61 5000 Namur Belgium
Dipartimento di Scienze Chimiche e Geologiche, Università di Cagliari, Complesso Universitario di Monserrato s.s. 554 Bivio per Sestu 09042 Monserrato CA Italy.
RSC Adv. 2018 Jul 16;8(45):25342-25350. doi: 10.1039/c8ra03878c.
Novel heterogeneous bi-functional catalysts bearing tin or zinc inserted as single sites within the silica architecture acting as acid centres and decorated with imidazolium moieties as the nucleophile source were successfully synthesized. The materials were extensively characterized various techniques including N physisorption, solid state nuclear magnetic resonance, X-ray photoelectron spectroscopy, transmission electron microscopy and adsorption microcalorimetry. The solids were tested as catalysts for the conversion of carbon dioxide, selecting the synthesis of styrene carbonate as the target reaction. Both materials exhibited improved performances compared to the analogous solids functionalized with the sole imidazolium salt as well as to other materials reported in the literature. The Sn-based catalyst displayed excellent conversion also in the presence of various epoxides. In all experiments the bi-functional solid allowed reducing the reaction temperature below 150 °C. In the presence of glycidol the temperature was decreased down to 30 °C. The short synthesis protocol of the heterogeneous catalysts, together with the 100% atom economy of the target reaction and the low reaction temperature, make the entire process highly sustainable. Moreover, the Sn-based catalyst was stable under the selected reaction conditions and reusable for multiple catalytic cycles.
成功合成了新型多相双功能催化剂,该催化剂在二氧化硅结构中作为酸中心插入锡或锌单原子位点,并以咪唑鎓部分作为亲核试剂源进行修饰。采用多种技术对材料进行了广泛表征,包括N物理吸附、固态核磁共振、X射线光电子能谱、透射电子显微镜和吸附量热法。将这些固体作为二氧化碳转化的催化剂进行测试,选择碳酸苯乙烯的合成作为目标反应。与仅用咪唑鎓盐功能化的类似固体以及文献中报道的其他材料相比,这两种材料均表现出更好的性能。在各种环氧化物存在的情况下,锡基催化剂也表现出优异的转化率。在所有实验中,双功能固体能够将反应温度降低至150℃以下。在缩水甘油存在的情况下,温度可降至30℃。多相催化剂简短的合成方案,以及目标反应100%的原子经济性和较低的反应温度,使得整个过程具有高度的可持续性。此外,锡基催化剂在选定的反应条件下稳定,可重复用于多个催化循环。