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Carbon Nanofibrous Microspheres Promote the Oxidative Double Carbonylation of Alkanes with CO
Chem ( IF 23.5 ) Pub Date : 2018-10-11 , DOI: 10.1016/j.chempr.2018.09.003
Lijun Lu , Xianglin Pei , Yuan Mei , Yi Deng , Heng Zhang , Lina Zhang , Aiwen Lei

Here, dual O- and N-doped carbon nanofibrous microspheres (CNMs) promoting the chemical transformation of alkane with CO have been achieved smoothly. Efficient conversion of bulk chemicals is of great significance in chemical synthesis. Carbonylation involving CO is an important process for constructing carbonyl compounds in industry and academia, among which stands out metal-catalyzed carbonylation. However, the strong coordination ability and reducibility of CO usually lower the activity of metal catalysts. Hence, it becomes urgent to explore novel conversion strategies, such as fabricating new materials to replace traditional catalysts. In this work, we show that chitin-derived CNMs mediate oxidative double carbonylation of alkanes for the preparation of various alkyl α-ketoamides. In our findings, the porous CNM with large surface area could supply potential adhesion sites for amines, which inhibited the oxidative decomposition of amines to promote this transformation. Notably, to our knowledge, oxidative double carbonylation of the alkane C(sp3)–H bond has not yet been reported.



中文翻译:

碳纳米纤维微球促进烷烃与CO的氧化双羰基化

在这里,已成功实现了O和N掺杂的碳纳米纤维双微球(CNM)促进烷烃与CO的化学转化。散装化学品的有效转化在化学合成中具有重要意义。涉及CO的羰基化是在工业界和学术界中构造羰基化合物的重要过程,其中金属催化的羰基化尤为突出。但是,CO的强配位能力和还原性通常会降低金属催化剂的活性。因此,迫切需要探索新颖的转化策略,例如制造新的材料来代替传统的催化剂。在这项工作中,我们表明,几丁质衍生的CNM介导烷烃的氧化双羰基化,以制备各种烷基α-酮酰胺。在我们的发现中,具有较大表面积的多孔CNM可以为胺提供潜在的粘附位点,从而抑制了胺的氧化分解,从而促进了这种转变。值得注意的是,据我们所知,烷烃C(sp3)–尚未报告H键。

更新日期:2018-10-11
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