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通过与晚期兰化物共价 δ-结合稳定的四基的线性反向三明治复合物

K Randall McClain¹, Alexandre H Vincent, Ahmadreza Rajabi²

¹US Navy, Naval Air Warfare Center, Weapons Division, Research Department, Chemistry Division, China Lake, California 93555, United States.

Journal of the American Chemical Society

|November 13, 2024

概括

合成了新的迪兰化逆三明治复合物,其中包括一种罕见的四基联体. 这些复合物表现出迄今为止观察到的最短的化物距离,展示了独特的结合相互作用.

科学领域:

有机金属化学
兰化物化学
协调化学

背景情况:

在催化和材料科学中,有机配体的兰化物复合物至关重要.
反向三明治复合体具有独特的电子和结构性质.
低价位有机配体的稳定通过兰坦化物是一个活跃的研究领域.

研究的目的:

合成和表征新的二甲逆三明治复合物.
研究这些独特化合物的结合和电子结构.
探索由兰他尼德稳定的一种四基联体的可能性.

主要方法:

通过减少三价兰二极体与石墨在的存在.
单晶X射线衍射用于结构确定.
频谱 (NMR,UV-Vis) 和磁性敏感性测量
用于电子结构分析的密度功能理论 (DFT) 计算.

主要成果:

对于Ln=Y,Gd,Tb,Dy,Tm,成功合成了二甲逆三明治复合物 (Cp^iPr5Ln) ₂:η⁶-C₆H₆.
通过X射线衍射证实了异常的线性协调几何和平面桥.
迄今为止观察到的最短的Ln-Bz_中心点距离 (1.943(1) Å对于Tm到2.039(6) Å对于Gd).
证据表明一种罕见的,未被替代的四基联体,通过强对应 δ 键稳定.

结论:

报告的化合物代表了具有未被替代的四基的后期化物复合物的第一个例子.
兰化物f轨道和化物π*轨道之间的强共价相互作用是稳定四离子联体的关键.
这些发现扩大了对化物和有机配体相互作用的理解,并在有机金属化学中开辟了新的途径.

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