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1,4-二硅苯的单电子和双电子转移氧化反应：稳定自由基阳离子和双阳离子的形成

One- and Two-Electron Transfer Oxidation of 1,4-Disilabenzene with Formation of Stable Radical Cations and Dications.

作者信息

Chen Yilin, Chen Zhikang, Jiang Liuyin, Li Jiancheng, Zhao Yiling, Zhu Hongping, Roesky Herbert W

机构信息

State Key Laboratory of Physical Chemistry of Solid Surfaces, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.

Institut für Anorganische Chemie, Georg-August-Universität, 37077, Göttingen, Germany.

出版信息

Chemistry. 2022 Jan 24;28(5):e202103715. doi: 10.1002/chem.202103715. Epub 2021 Dec 16.

DOI:10.1002/chem.202103715
PMID:34837718
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9299862/
Abstract

Electron-transferable oxidants such as B(C F ) /nBuLi, B(C F ) /LiB(C F ) , B(C F ) /LiHBEt , Al(C F ) /(o-RC H )AlH (R=N(CMe CH ) CH ), B(C F ) /AlEt , Al(C F ) , Al(C F ) /nBuLi, Al(C F ) /AlMe , (CuC F ) , and Ag SO , respectively were employed for reactions with (L) Si C (SiMe ) (C SiMe ) (L=PhC(NtBu) , 1). The stable radical cation [1] was formed and paired with the anions [nBuB(C F ) ] (in 2), [B(C F ) ] (in 3), [HB(C F ) ] (in 4), [EtB(C F ) ] (in 5), {[(C F ) Al] (μ-F)] (in 6), [nBuAl(C F ) ] (in 7), and [Cu(C F ) ] (in 8), respectively. The stable dication [1] was also generated with the anions [EtB(C F ) ] (9) and [MeAl(C F ) ] (10), respectively. In addition, the neutral compound [(L) Si C (SiMe ) (C SiMe ) ][μ-O S(O) ] (11) was obtained. Compounds 2-11 are characterized by UV-vis absorption spectroscopy, X-ray crystallography, and elemental analysis. Compounds 2-8 are analyzed by EPR spectroscopy and compounds 9-11 by NMR spectroscopy. The structure features are discussed on the central Si C -rings of 1, [1] , [1] , and 11, respectively.

摘要

分别使用可进行电子转移的氧化剂，如B(C₆F₅)₃/nBuLi、B(C₆F₅)₃/LiB(C₆F₅)₄、B(C₆F₅)₃/LiHBEt₃、Al(C₆F₅)₃/(o-RC₆H₄)₂AlH₂(R = N(CMe₂CH₂)₂CH₂)、B(C₆F₅)₃/AlEt₃、Al(C₆F₅)₃、Al(C₆F₅)₃/nBuLi、Al(C₆F₅)₃/AlMe₃、(CuC₆F₅)₂和Ag₂SO₄，与(L)SiC(SiMe₃)(C₂SiMe₃)(L = PhC(NtBu)₂, 1)进行反应。形成了稳定的自由基阳离子[1]，并分别与阴离子[nBuB(C₆F₅)₄]（在2中）、[B(C₆F₅)₄]（在3中）、[HB(C₆F₅)₃]（在4中）、[EtB(C₆F₅)₃]（在5中）、{(C₆F₅)₂Al}（在6中）、[nBuAl(C₆F₅)₃]（在7中）和[Cu(C₆F₅)₂]（在8中）配对。稳定的二价阳离子[1]也分别与阴离子[EtB(C₆F₅)₃]（9）和[MeAl(C₆F₅)₃]（10）生成。此外，还得到了中性化合物[(L)SiC(SiMe₃)(C₂SiMe₃)][μ-O₂S(O)₂]（11）。化合物2 - 11通过紫外 - 可见吸收光谱、X射线晶体学和元素分析进行表征。化合物2 - 8通过电子顺磁共振光谱分析，化合物9 - 11通过核磁共振光谱分析。分别讨论了1、[1]⁺、[1]²⁺和11的中心SiC - 环的结构特征。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a2cb/9299862/e100d995db72/CHEM-28-0-g010.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a2cb/9299862/14cbfa1ec99f/CHEM-28-0-g009.jpg
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