Multielectron Reduction of Nitrosoarene via Aluminylene-Silylene Cooperation

IF 14.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Journal of the American Chemical Society Pub Date : 2024-10-17 DOI:10.1021/jacs.4c10323
Xi Chen, Dezhi Yang, Fanshu Cao, Zhenbo Mo
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Abstract

The cooperative effects of main-group elements pave the way for novel chemical transformations. However, the potential of bimetallic complexes featuring the most abundant aluminum and silicon elements remains largely unexplored. In this study, we present the synthesis and characterization of bis(silylene)-stabilized aluminylene 2. The cooperation between aluminylene and silylene allows for the facile cleavage of the N–O bond in nitrosoarenes, producing an aluminum imide complex 4 and tetracyclic oxazasilaalanes 5 and 6, and also promotes the dearomatization of 2-methylquinoline, yielding a silylalane 7. In addition, 2 is an effective precatalyst for the reductive coupling of nitrosoarenes to azoxyarenes. These results outline an approach for orchestrating aluminum and silicon cooperation to facilitate chemical bond activation.

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通过铝-硅合作实现亚硝基炔的多电子还原
主族元素的协同效应为新型化学转化铺平了道路。然而,以最丰富的铝元素和硅元素为特征的双金属复合物的潜力在很大程度上仍未得到开发。在本研究中,我们介绍了双(硅烷基)稳定铝烯 2 的合成和表征。铝烯和硅烯之间的合作使得亚硝基烯烃中的 N-O 键易于裂解,从而生成铝亚胺络合物 4 以及四环噁唑硅烷 5 和 6,还能促进 2-甲基喹啉的脱芳烃化,生成硅烷 7。此外,2 还是一种有效的前催化剂,可将亚硝基烯烃还原偶联为氮氧烯烃。这些结果概述了一种协调铝和硅合作以促进化学键活化的方法。
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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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