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磺酸酯 N-杂环卡宾-铜配合物:手性合成 C-C、C-B、C-H 和 C-Si 键的高效独特催化剂。

Sulfonate N-Heterocyclic Carbene-Copper Complexes: Uniquely Effective Catalysts for Enantioselective Synthesis of C-C, C-B, C-H, and C-Si Bonds.

机构信息

Department of Chemistry, Merkert Chemistry Center, Boston College, Chestnut Hill, MA, 02467, USA.

Supramolecular Science and Engineering Institute, University of Strasbourg, CNRS, 67000, Strasbourg, France.

出版信息

Angew Chem Int Ed Engl. 2020 Nov 23;59(48):21304-21359. doi: 10.1002/anie.202003755. Epub 2020 Aug 26.

Abstract

A copper-based complex that contains a sulfonate N-heterocyclic carbene ligand was first reported 15 years ago. Since then, these organometallic entities have proven to be uniquely effective in catalyzing an assortment of enantioselective transformations, including allylic substitutions, conjugate additions, proto-boryl additions to alkenes, boryl and silyl substitutions, hydride-allyl additions to alkenyl boronates, and additions of boron-containing allyl moieties to N-H ketimines. In this review article, we detail the shortcomings in the state-of-the-art that fueled the development of this air stable ligand class, members of which can be prepared on multigram scale. For each reaction type, when relevant, the prior art at the time of the advance involving sulfonate NHC-Cu catalysts and/or subsequent key developments are briefly analyzed, and the relevance of the advance to efficient and enantioselective total or formal synthesis of biologically active molecules is underscored. Mechanistic analysis of the structural attributes of sulfonate NHC-Cu catalysts that are responsible for their ability to facilitate transformations with high efficiency as well as regio- and enantioselectivity are detailed. This review contains several formerly undisclosed methodological advances and mechanistic analyses, the latter of which constitute a revision of previously reported proposals.

摘要

一种含有磺酸盐 N-杂环卡宾配体的铜基配合物是在 15 年前首次报道的。自那时以来,这些有机金属实体已被证明在催化各种对映选择性转化方面非常有效,包括烯丙基取代、共轭加成、烯属 proto-boryl 加成、硼基和硅基取代、烯基硼酸酯的氢-烯丙基加成以及含硼烯丙基部分向 N-H 酮亚胺的加成。在这篇综述文章中,我们详细介绍了推动这种空气稳定配体类发展的最新技术的不足之处,其中的成员可以在多克规模上制备。对于每种反应类型,在相关情况下,简要分析了涉及磺酸盐 NHC-Cu 催化剂的先有技术以及随后的关键发展,并且强调了该进展对生物活性分子的高效和对映选择性全合成或形式合成的相关性。详细说明了对磺酸盐 NHC-Cu 催化剂的结构属性的机制分析,这些属性负责其能够高效、区域和对映选择性地促进转化的能力。本综述包含了几个以前未公开的方法学进展和机制分析,后者构成了对以前报道的建议的修订。

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