Abstract A set of heteropolyacid-based ionic heterogeneous catalysts (PW@IL-GO(m)) have been synthesized by intercalated heteropolyanions in ionic liquid (IL)-functionalized graphene oxide (GO) via amino-protonation and/or anion-exchange reaction. This immobilization method offered improved dispersity, accessibility and stability of active sites. The amphipathic nature of IL-GO sheets and porosity of PW@IL-GO(m) are beneficial to reducing mass transfer limitation in a water/organic substrate two-phase system. Then, these obtained hybrids were employed as efficient and robust catalysts for the selective oxidation of alcohols into carbonyl compounds using hydrogen peroxide as an oxidant under organic solvent-free condition. As expected, PW@IL-GO(m) catalysts showed even much better activity than the corresponding homogeneous HPW (phosphotungstic acid) catalyst. Particularly, PW@IL-GO(1.5) gave a benzyl alcohol conversion of 94% and benzaldehyde chemoselectivity of 91%. Moreover, owing to the heterogeneous nature and strong cation–anion interactions between cationic supporter and PW anions, the as-prepared catalyst presented advantages of convenient recovery, simple preparation and steady reuse, further providing the industrial application potential in sustainable oxidation reactions.

中文翻译：

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插入离子液体功能化氧化石墨烯中的强杂多阴离子催化 H2O2 选择性氧化醇

摘要 通过氨基质子化和/或阴离子交换反应在离子液体 (IL) 功能化氧化石墨烯 (GO) 中插入杂多阴离子，合成了一套基于杂多酸的离子多相催化剂 (PW@IL-GO(m))。 . 这种固定方法提高了活性位点的分散性、可及性和稳定性。IL-GO 片的两亲性质和 PW@IL-GO(m) 的孔隙率有利于减少水/有机基质两相系统中的传质限制。然后，将这些获得的杂化物用作有效且稳健的催化剂，用于在无有机溶剂条件下使用过氧化氢作为氧化剂将醇选择性氧化成羰基化合物。正如预期的那样，PW@IL-GO(m) 催化剂比相应的均相 HPW（磷钨酸）催化剂表现出更好的活性。特别是，PW@IL-GO(1.5) 的苯甲醇转化率为 94%，苯甲醛化学选择性为 91%。此外，由于阳离子载体和 PW 阴离子之间的非均相性和强阳离子 - 阴离子相互作用，所制备的催化剂具有回收方便、制备简单和稳定重复利用的优点，进一步提供了可持续氧化反应的工业应用潜力。