Modular Polyoxometalate–Layered Double Hydroxides as Efficient Heterogeneous Sulfoxidation and Epoxidation Catalysts
Modular Polyoxometalate–Layered Double Hydroxides as Efficient Heterogeneous Sulfoxidation and Epoxidation Catalysts
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DOI：
10.1002/cctc.201701056
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发表时间：
2018-01
期刊：
影响因子：
4.5
通讯作者：
Tengfei Li;Wei Zhang;Wei Chen-;H. Miras;Yu‐Fei Song
中科院分区：
文献类型：
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作者：
Tengfei Li;Wei Zhang;Wei Chen-;H. Miras;Yu‐Fei Song
硫化物的选择性亚砜化和烯烃的选择性环氧化是两类重要的有机反应，相应的亚砜、砜和环氧化物的产物在工业生产中被广泛用作原料。为这两种反应制造一种有效的催化剂仍然是一项具有挑战性的任务。我们报道了一种高效的非均相催化剂Mg3Al‐ILs‐La(PW11)2的制备方法。通过FT - IR光谱、XRD、热重和差热分析、BET测量、X射线光电子能谱、29Si交叉极化魔角自旋核磁共振光谱、27Al魔角自旋核磁共振光谱、SEM、高分辨率TEM和能量色散X射线光谱对催化剂进行了表征。所设计的催化剂在温和条件下对硫化物的亚砜化反应和烯烃的环氧化反应具有较高的效率和选择性，产率分别为208和31 mmol g−1 h−1。此外，Mg3Al - il - La(PW11)2可以循环使用至少5次而不明显降低其催化活性。放大后的实验表明，该催化剂保持了其高效和稳健性，证明了该催化剂在工业应用中的巨大潜力。
The selective sulfoxidation of sulfides and the epoxidation of olefins are two types of important organic reactions, and the corresponding products of sulfoxides, sulfones and epoxides are used widely as raw materials in industrial processes. The fabrication of one efficient catalyst for both reactions remains a challenging task. We report the preparation of a highly efficient heterogeneous catalyst Mg3Al‐ILs‐La(PW11)2 using an exfoliation/assembly approach. The catalyst was characterised by FT‐IR spectroscopy, XRD, thermogravimetric and differential thermal analysis, BET measurements, X‐ray photoelectron spectroscopy, 29Si cross‐polarisation magic‐angle spinning NMR spectroscopy, 27Al magic‐angle spinning NMR spectroscopy, SEM, high‐resolution TEM, and energy‐dispersive X‐ray spectroscopy. The designed catalyst showed a high efficiency and selectivity for the sulfoxidation of sulfides and the epoxidation of olefins under mild conditions at a production rate of 208 and 31 mmol g−1 h−1, respectively. Moreover, Mg3Al‐ILs‐La(PW11)2 can be recycled and re‐used at least five times without a clear decrease of its catalytic activity. The scaled‐up experiments revealed that the catalyst retained its efficiency and robustness, which demonstrates the great potential of the catalyst for industrial applications.