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一个双质的反 (iii) / (iii) 挫败了易斯对

Jonas Krieft¹, Pia C Trapp¹, Yury V Vishnevskiy¹

¹Chair of Inorganic and Structural Chemistry, Center for Molecular Materials CM2, Faculty of Chemistry, Bielefeld University, Universitätsstraße 25 Bielefeld 33615 Germany mitzel@uni-bielefeld.de.

Chemical science

|August 2, 2024

概括

一个新的双胞胎路易斯对, (F5C2) 2SbCH2P(tBu) 2,由于其柔软的反中心,与CS2等小分子表现出独特的反应性. 这个易斯对表现出FLP类型的行为,与各种化合物形成 adducts.

科学领域:

有机金属化学有机金属化学
主群化学化学
超分子化学超分子化学

背景情况:

易斯对的合成和反应性对于开发新的催化系统至关重要.
了解易斯酸性中心的电子性质,即使具有高度电负替代物,也是预测反应性的关键.
与传统的易斯酸和相比,双子易斯对具有独特的结构和电子特性.

研究的目的:

为了合成和描述一个新的双胞胎路易斯对, (F5C2) 2SbCH2P(tBu) 2 (1).
为了研究化合物1中的中心的易斯酸性质,特别是与HSAB概念相关.
探索化合物1与小分子和异构素的反应性,包括其作为丧的易斯对 (FLP) 的潜力.

主要方法:

通过 (F5C2) 2SbCl与LiCH2P (tBu) 2反应合成 (F5C2) 2SbCH2P (tBu) 2 (1) 通过 (F5C2) 2SbCl与LiCH2P (tBu) 2的反应合成.
使用VT-NMR光谱来研究可逆CS2结合的表征.
量子化学计算 (DFT,QTAIM,IQA) 用于分析反应机制和电子结构.
用X射线衍射,多核核核磁共振和元素分析进行结构和组成验证.

主要成果:

化合物1,尽管具有高度负电子的替代物,但呈现出柔软的易斯酸性反中心.
观察到CS2与化合物1的可逆结合,而CO2没有反应.
与SO2,PhNCO,PhNCS和 (MePh2P) AuCl表现出FLP类型的反应性,形成各种添加物和循环产物.
形成了一个与 (MePh2P) AuCl 形成的独特的状添加物,由两个原子对化离子进行化.

结论:

双易斯对 (F5C2) 2SbCH2P(tBu) 2显示可调的易斯酸度和多功能反应性.
它的柔软的易斯酸性质使其能够与像CS2这样的小分子进行特定的相互作用.
该化合物作为探索FLP化学和设计新型有机金属复合物的宝贵平台.

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