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Imidazolium-based titanosilicate nanospheres as active catalysts in carbon dioxide conversion: Towards a cascade reaction from alkenes to cyclic carbonates
Journal of CO2 Utilization ( IF 7.7 ) Pub Date : 2021-04-16 , DOI: 10.1016/j.jcou.2021.101529
Adrien Comès , Rémy Poncelet , Paolo P. Pescarmona , Carmela Aprile

Porous silica-based nanospheres bearing titanium centres as single site were successfully synthesized employing a time- and energy-efficient procedure. The influence of the post-synthesis treatment on the insertion of Ti was investigated via DR UV–Vis and XPS spectroscopy and the titanium content was quantified through ICP-OES analysis. The textural and structural properties of the different solids were evaluated via XRD, TEM and N2 physisorption. The resulting materials were thereafter covalently functionalized with imidazolium chloride, followed by characterization via 29Si and 13C solid-state NMR, N2 physisorption and chemical combustion analysis. The bi-functional catalysts were tested in the challenging conversion of CO2 with cyclohexene oxide to the corresponding cyclic carbonate as well as with various other epoxides with excellent results. The insertion of Ti as single site played a key role substantially improving the activity of the solids. The most active bi-functional material was successfully recovered and reused through multiple cycle without loss of the catalytic activity. Moreover, the cyclohexene epoxidation reaction was tested as well employing the mono-functionalized Ti-based material. The catalytic mixture, composed by the mono-functional and bi-functional solids, was efficiently used to convert the cyclohexene into cyclohexene oxide and subsequently the cyclohexene oxide into the corresponding carbonate thus opening the prospect for a cascade reaction.



中文翻译:

基于咪唑鎓的钛硅酸盐纳米球作为二氧化碳转化中的活性催化剂:实现从烯烃到环状碳酸酯的级联反应

以时间和能源效率高的程序成功合成了以钛中心为单个位点的多孔二氧化硅基纳米球。通过DR UV-Vis和XPS光谱研究了合成后处理对Ti插入的影响,并通过ICP-OES分析定量了钛的含量。通过XRD,TEM和N 2物理吸附评估了不同固体的质地和结构性质。然后将所得材料与咪唑氯化物共价官能化,然后通过29 Si和13 C固态NMR,N 2物理吸附和化学燃烧分析进行表征。在具有挑战性的CO转化率中测试了双功能催化剂2与氧化环己烯为相应的环状碳酸酯,以及与具有优良的结果的各种其他环氧化物。Ti作为单个位点的插入起了关键作用,大大提高了固体的活性。活性最高的双功能材料已成功回收并通过多个循环重复使用,而不会损失催化活性。此外,也使用单官能化的Ti基材料测试了环己烯的环氧化反应。由单官能和双官能固体组成的催化混合物可有效地用于将环己烯转化为环己烯氧化物,然后将环己烯氧化物转化为相应的碳酸酯,从而为级联反应开辟了前景。

更新日期:2021-04-16
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