C-H活化1,5-镍迁移和C-Si活化1,4-镍迁移在镍催化下合成硅烷

IF 11.3 1区 化学 Q1 CHEMISTRY, PHYSICAL
Donghyeon Lee, Ikuya Fujii, Ryo Shintani
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引用次数: 0

摘要

涉及1,n-金属迁移的催化反应为通过激活非反应键从简单前体合成复杂分子骨架提供了一种强有力的方法。在本研究中,通过C-H键激活1,5-镍迁移和C-Si键激活1,4-镍迁移的反应,镍催化合成了3,3-二取代1-硅烷,这是一种有价值的硅烷的硅类似物。研究发现,1,5-镍的迁移不仅使C-H键在较远的位置活化,而且控制了随后插入烯烃的区域选择性。通过氘标记实验和DFT计算对反应机理进行了详细研究。本研究结果表明,通过C-H和C-Si键活化镍迁移的催化反应在合成有用的环有机硅化合物中具有很高的潜力。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Nickel-Catalyzed Synthesis of Silaindanes via Sequential C–H Activating 1,5-Nickel Migration and C–Si Activating 1,4-Nickel Migration

Nickel-Catalyzed Synthesis of Silaindanes via Sequential C–H Activating 1,5-Nickel Migration and C–Si Activating 1,4-Nickel Migration
Catalytic reactions involving 1,n-metal migration provide a powerful approach for the synthesis of complex molecular skeletons from simple precursors through the activation of unreactive bonds. In this work, a nickel-catalyzed synthesis of 3,3-disubstituted 1-silaindanes, silicon analogues of valuable indanes, was developed by the reaction involving 1,5-nickel migration via C–H bond activation and 1,4-nickel migration via C–Si bond activation. It was found that 1,5-nickel migration not only enabled the C–H bond activation at a remote position but also controlled the regioselectivity of subsequent alkene insertion. The detailed reaction mechanism was investigated by conducting deuterium labeling experiments and DFT calculations. The results obtained here demonstrate the high potential of catalytic reactions involving nickel migrations via C–H and C–Si bond activations for the synthesis of useful cyclic organosilicon compounds.
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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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