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最新的 C-H 功能化与 C-C 断裂偶联合成方法学进展。

Recent Advances on Synthetic Methodology Merging C-H Functionalization and C-C Cleavage.

机构信息

Department of Chemistry, Faculty of Science, Ferdowsi University of Mashhad, Mashhad 91775-1436, Iran.

Grupo de Química Organometálica, Campus de Espinardo, Universidad de Murcia, 30100 Murcia, Spain.

出版信息

Molecules. 2020 Dec 13;25(24):5900. doi: 10.3390/molecules25245900.

DOI:10.3390/molecules25245900
PMID:33322116
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC7764206/
Abstract

The functionalization of C-H bonds has become a major thread of research in organic synthesis that can be assessed from different angles, for instance depending on the type of catalyst employed or the overall transformation that is carried out. This review compiles recent progress in synthetic methodology that merges the functionalization of C-H bonds along with the cleavage of C-C bonds, either in intra- or intermolecular fashion. The manuscript is organized in two main sections according to the type of substrate in which the cleavage of the C-C bond takes place, basically attending to the scission of strained or unstrained C-C bonds. Furthermore, the related research works have been grouped on the basis of the mechanistic aspects of the different transformations that are carried out, i.e.,: (a) classic transition metal catalysis where organometallic intermediates are involved; (b) processes occurring via radical intermediates generated through the use of radical initiators or photochemically; and (c) reactions that are catalyzed or mediated by suitable Lewis or Brønsted acid or bases, where molecular rearrangements take place. Thus, throughout the review a wide range of synthetic approaches show that the combination of C-H and C-C cleavage in single synthetic operations can serve as a platform to achieve complex molecular skeletons in a straightforward manner, among them interesting carbo- and heterocyclic scaffolds.

摘要

C-H 键的功能化已成为有机合成的主要研究课题,可以从不同角度进行评估,例如取决于所采用的催化剂类型或进行的整体转化。本综述汇集了最近在合成方法学方面的进展,该方法将 C-H 键的功能化与 C-C 键的断裂结合在一起,无论是在分子内还是分子间方式。根据 C-C 键断裂发生在何种类型的底物中,本文主要分为两个部分,基本上是针对张力或无张力 C-C 键的断裂。此外,根据所进行的不同转化的机理方面,将相关的研究工作进行了分组,即:(a)经典的过渡金属催化,其中涉及有机金属中间体;(b)通过使用自由基引发剂或光化学产生自由基中间体而发生的过程;和(c)由合适的路易斯酸或布朗斯台德酸或碱催化或介导的反应,其中发生分子重排。因此,在整个综述中,广泛的合成方法表明,在单个合成操作中 C-H 和 C-C 断裂的组合可以作为一种平台,以直接的方式实现复杂的分子骨架,其中包括有趣的碳和杂环支架。

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