Liu Xueting, Li Daojing, Li Guoao, Wei Mengran, Yuan Shihao, Yang Mo, He Linke, Chen Shengda, Li Zhenxing, Gao Liuzhou, Wang Guoqiang, Li Shuhua
State Key Laboratory of Coordination Chemistry, Key Laboratory of Mesoscopic Chemistry of Ministry of Education, School of Chemistry and Chemical Engineering, New Cornerstone Science Laboratory, Nanjing University, Nanjing, P. R. China.
School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, P. R. China.
Nat Commun. 2025 Jul 1;16(1):5458. doi: 10.1038/s41467-025-60674-9.
Organometallic reagents are essential tools in both academic and industrial laboratories and the polarity separation within the carbon-metal bonds endows them with exceptional reactivities, but also imposes limitations, including air- and moisture-sensitivity, and flammability. Here, we demonstrate that stable and easily accessible benzylic (or allylic) boronate with alkali-metal alkoxide as the activator can act as reactive organometallic reagents. This strategy enables transition metal-free deprotonative C-H borylation of diverse (hetero)arenes. The polar organometallic nature of this process enables predictable and site-selective borylation by targeting the arenes's most acidic C-H bond. This approach can be coupled with Suzuki-Miyaura reaction to produce C-H arylation products. We have also applied this strategy to the dehalogenative borylation of aryl bromides and anionic polymerization of styrenes. Given the unique stability and structural diversity of organoboronates, their organometallic-type reactivities show promise as a powerful alternative to synthetic methodologies that rely on sensitive organometallic reagents.
有机金属试剂是学术和工业实验室中必不可少的工具,碳 - 金属键内的极性分离赋予它们非凡的反应活性,但也带来了局限性,包括对空气和水分敏感以及易燃性。在这里,我们证明了以碱金属醇盐为活化剂的稳定且易于获得的苄基(或烯丙基)硼酸酯可以作为活性有机金属试剂。该策略能够实现多种(杂)芳烃的无过渡金属去质子化C - H硼化反应。这一过程的极性有机金属性质通过靶向芳烃中最酸性的C - H键实现了可预测的位点选择性硼化反应。该方法可与铃木 - 宫浦反应偶联以生成C - H芳基化产物。我们还将此策略应用于芳基溴的脱卤硼化反应和苯乙烯的阴离子聚合反应。鉴于有机硼酸酯独特的稳定性和结构多样性,它们的有机金属型反应活性有望成为依赖敏感有机金属试剂的合成方法的有力替代方案。