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A general and highly regioselective synthesis approach to multi-functionalized organoimido derivatives of Polyoxometalates

机译:一种多金属氧酸酯的多功能有机亚氨基衍生物的通用且高度区域选择性的合成方法

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摘要

Organoimidoylization of Polyoxometalates (POMs) can dramatically modify the electronic structures of POMs and gives rise to novel “value-adding” properties of the POMs for promising material applications including photo-electronic transformation and catalysis. To date, the preparation of multi-functionalized organoimido derivatives of POMs is generally conducted under strict condition and is time-consuming with limited yields. Herein, a series of regioselective polyorganoimido derivatives of POMs, ocatant- [Mo6O13(NAr)3(μ2-NAr)3]2>− (Ar = phenyl (>1), p-methoxyphenyl (>2) and p-ethylphenyl (>3)), were synthesized with high selectivity and in good yields via a general and highly regioselective synthesis method, called as the one-octant synthesis protocol. The reaction was monitored by ESI-MS and the as-prepared products were studied by ESI-MS, IR, UV-Vis, EA, 1HNMR, single crystal XRD analysis and DFT calculations. The one-octant synthesis protocol here may serve as an idea method to design novel nanoscale POM-based organic-inorganic multi-functional hybrids.
机译:多金属氧酸盐(POM)的有机酰胺化可以极大地改变POM的电子结构,并为具有前景的材料应用(包括光电转换和催化)带来新颖的“增值”特性。迄今为止,POM的多功能有机亚胺衍生物的制备通常在严格条件下进行,并且费时且产率有限。在此,列出了一系列POM的区域选择性聚有机亚氨基衍生物,即-[Mo6O13(NAr)3(μ2-NAr)3] 2 >- (Ar =苯基(> 1 ),对甲氧基苯基(> 2 )和对乙苯基(> 3 ))的合成具有很高的选择性和高收率。区域选择性合成方法,称为一八分之一合成协议。通过ESI-MS监测反应,并通过ESI-MS,IR,UV-Vis,EA, 1 HNMR,单晶XRD分析和DFT计算研究所制备的产物。这里的一个八分位数合成协议可以用作设计新颖的基于纳米级POM的有机-无机多功能杂化物的方法。

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