镍催化的甲酰胺的苄位 β-C(sp 3 )-H 键活化。
Ni-catalyzed benzylic β-C(sp)-H bond activation of formamides.
机构信息
State Key Laboratory and Institute of Elemento-Organic Chemistry, College of Chemistry, Nankai University, Tianjin, 300071, China.
Department of Chemistry, School of Science and Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Tianjin University, Tianjin, 300072, China.
出版信息
Nat Commun. 2022 Dec 22;13(1):7892. doi: 10.1038/s41467-022-35541-6.
The development of transition metal-catalyzed β-C-H bond activation via highly-strained 4-membered metallacycles has been a formidable task. So far, only scarce examples have been reported to undergo β-C-H bond activation via 4-membered metallacycles, and all of them rely on precious metals. In contrast, earth-abundant and inexpensive 3d transition metal-catalyzed β-C-H bond activation via 4-membered metallacycles still remains an elusive challenge. Herein, we report a phosphine oxide-ligated Ni-Al bimetallic catalyst to activate secondary benzylic C(sp)-H bonds of formamides via 4-membered nickelacycles, providing a series of α,β-unsaturated γ-lactams in up to 97% yield.
通过高度应变的四元金属环来实现过渡金属催化的β-C-H 键活化一直是一项艰巨的任务。到目前为止，只有少数报道的例子通过四元金属环经历了β-C-H 键活化，而且它们都依赖于贵金属。相比之下，通过四元金属环实现丰富且廉价的 3d 过渡金属催化的β-C-H 键活化仍然是一个难以实现的挑战。在此，我们报告了一种磷氧化物配体的 Ni-Al 双金属催化剂，通过四元镍环来激活甲酰胺的仲苄基 C(sp)-H 键，以高达 97%的收率提供了一系列α,β-不饱和γ-内酰胺。
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