配体催化镍催化具有多种原生官能团的烯烃的二羧官能化反应

IF 14.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Nature Communications Pub Date : 2024-11-28 DOI:10.1038/s41467-024-54170-9
Dao-Ming Wang, Hui-Mei Shan, Li-Qin She, Yu-Qing He, Yichen Wu, Yong Tang, Li-Ping Xu, Peng Wang
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引用次数: 0

摘要

过渡金属催化的未活化烯烃二羧官能化通常需要外源强配位定向基团,从而降低了整体反应效率。在此,我们报告了一种配体催化的 Ni(II) 二羧官能化技术,该技术以芳基/烯基硼酸和烷基卤化物为偶联剂,以多种原生官能团为指导基团,对未活化的烯烃进行二羧官能化。在氧化还原中性条件下,使用传统方法难以获得的伯、仲、叔酰胺、磺酰胺以及仲胺和叔胺,这种二羧官能化协议提供了一条高效、直接的途径,可以制备邻位 1,2 二取代烷烃。这一反应成功的关键在于使用了笨重的 β-二酮配体,它可以使烯插入芳基-Ni(II) 物种,稳定烷基-Ni(II) 物种,并抑制烷基-Ni(II) 的同源裂解,实验和计算研究都证明了这一点。这种二羧基官能化反应具有使用原生定向基团、底物范围广和良好的可扩展性等特点。
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Ligand-enabled Ni-catalysed dicarbofunctionalisation of alkenes with diverse native functional groups

The transition metal-catalysed dicarbofunctionalisation of unactivated alkenes normally requires exogenous strong coordinated directing groups, thus reducing the overall reaction efficiency. Here, we report a ligand-enabled Ni(II)-catalysed dicarbofunctionalisation of unactivated alkenes with aryl/alkenyl boronic acids and alkyl halides as the coupling partners with a diverse range of native functional groups as the directing group. This dicarbofunctionalisation protocol provides an efficient and direct route towards vicinal 1,2-disubstituted alkanes using primary, secondary, tertiary amides, sulfonamides, as well as secondary and tertiary amines under redox-neutral conditions that are challenging to access through conventional methods. The key to the success of this reaction is the use of a bulky β-diketone ligand, which could enable the insertion of alkene to aryl-Ni(II) species, stabilize the alkyl-Ni(II) species and inhibit the homolytic alkyl-Ni(II) cleavage, supporting by both experimental and computational studies. This dicarbofunctionalisation reaction features the use of native directing group, a broad substrate scope, and excellent scalability.

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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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