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Metal-Ligand Core-Shell Nanocomposite Catalysts for the Selective Semihydrogenation of Alkynes

机译:金属配体核壳纳米复合催化剂对炔烃的选择性半加氢反应

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摘要

In recent years, hybrid nanocomposites with core-shell structures have increasingly attracted enormous attention in many important research areas such as quantum dots, optical, magnetic, and electronic devices, and catalysts. In the catalytic applications of core-shell materials, core-metals having magnetic properties enable easy separation of the catalysts from the reaction mixtures by a magnet. The core-metals can also affect the active shell-metals, delivering significant improvements in their activities and selectivities. However, it is difficult for core-metals to act directly as the catalytic active species because they are entirely covered by the shell. Thus, few successful designs of core-shell nanocomposite catalysts having active metal species in the core have appeared to date. Recently, we have demonstrated the design of a core-shell catalyst consisting of active metal nanoparticles (NPs) in the core and closely assembled oxides with nano-gaps in the shell, allowing the access of substrates to the core-metal. The shell acted as a macro ligand (shell ligand) for the core-metal and the core-shell structure maximized the metal-ligand interaction (ligand effect), promoting highly selective reactions.' The design concept of core-shell catalysts having core-metal NPs with a shell ligand is highly useful for selective organic transformations owing to the ideal structure of these catalysts for maximizing the ligand effect, leading to superior catalytic performances compared to those of conventional supported metal NPs.
机译:近年来,具有核-壳结构的杂化纳米复合材料在许多重要的研究领域(例如量子点,光学,磁性和电子设备以及催化剂)越来越引起人们的极大关注。在核-壳材料的催化应用中,具有磁性的核-金属能够通过磁体容易地将催化剂与反应混合物分离。芯金属还可以影响活性壳金属,从而显着改善其活性和选择性。但是,芯金属很难直接充当催化活性物质,因为它们被壳层完全覆盖。因此,迄今为止,几乎没有成功设计出在芯中具有活性金属物质的芯-壳纳米复合催化剂。最近,我们已经展示了一种核-壳催化剂的设计,该核-壳催化剂由核中的活性金属纳米颗粒(NPs)和紧密组装的氧化物以及壳中具有纳米间隙的氧化物组成,从而使基材可以进入核金属。壳充当核金属的大配体(壳配体),并且核-壳结构最大化了金属-配体相互作用(配体效应),从而促进了高度选择性的反应。具有带壳配体的核金属NP的核-壳催化剂的设计理念对选择性有机转化非常有用,这是因为这些催化剂具有理想的结构,可最大程度地发挥配体效应,与常规负载金属相比,具有卓越的催化性能NP。

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