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Rational design of a polyoxometalate intercalated layered double hydroxide: highly efficient catalytic epoxidation of allylic alcohols under mild and solvent-free conditions

机译:多金属氧酸盐嵌入层状双氢氧化物的合理设计:在温和无溶剂条件下高效催化环氧化烯丙醇

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摘要

Intercalation catalysts, owing to their modular and accessible gallery and unique interlamellar chemical environment, have shown wide application in various catalytic reactions. However, the poor mass transfer between the active components of the intercalated catalysts and organic substrates is one of the challenges that limit their further application. Herein, we have developed a novel heterogeneous catalyst by intercalating the polyoxometalate (POM) of Na9LaW10O36⋅32 H2O (LaW10) into layered double hydroxides (LDHs), which have been covalently modified with ionic liquids (ILs). The intercalation catalyst demonstrates high activity and selectivity for the epoxidation of various allylic alcohols in the presence of H2O2. For example, trans-2-hexen-1-ol undergoes up to 96 % conversion and 99 % epoxide selectivity at 25 °C in 2.5 h. To the best of our knowledge, the Mg3Al−ILs−C8−LaW10 composite material constitutes one of the most efficient heterogeneous catalysts for the epoxidation of allylic alcohols (including the hydrophobic allylic alcohols with long alkyl chains) reported so far.
机译:插层催化剂由于其模块化且易于接近的通道和独特的层间化学环境,已在各种催化反应中得到了广泛的应用。然而,插层催化剂的活性组分与有机底物之间的不良传质是限制其进一步应用的挑战之一。本文中,我们通过将Na9LaW10O36⋅32H2O(LaW10)的多金属氧酸盐(POM)插入层状双氢氧化物(LDHs)中,将其插入离子液体(ILs)进行共价改性,从而开发了一种新型的非均相催化剂。在H2O2存在下,插层催化剂对各种烯丙基醇的环氧化表现出高活性和选择性。例如,反式-2-己烯-1-醇在25°C下2.5?h内可达到96%的转化率和99%的环氧选择性。据我们所知,Mg3Al-ILs-C8-LaW10复合材料是迄今为止报道的烯丙基醇(包括具有长烷基链的疏水烯丙基醇)环氧化的最有效的多相催化剂之一。

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