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主群分子中的分散力和反直觉的固体效应:更重的14组 (Si-Pb) 二基酸碳类型,具有90°以下的交联键结合角度

Brian D Rekken¹, Thomas M Brown, James C Fettinger

¹Department of Chemistry, University of California, Davis, One Shields Avenue, Davis, California, 95616, USA.

Journal of the American Chemical Society

|June 4, 2013

概括

研究人员合成了具有不寻常的急性结合角度的四二基酸盐. 这些角度,与固态预期相反,随着连接体大小的增加而变窄,被分散力稳定.

科学领域:

有机金属化学有机金属化学
主群化学化学
无机合成无机合成

背景情况:

四烯 (Si,Ge,Sn,Pb) 通常与体积大的配体一起研究以控制反应性.
单质二二甲基酸盐 (M(ChAr) 2) 为探索结合和结构性质提供了一个独特的平台.
了解影响这些化合物的键角的因素对于预测它们的行为至关重要.

研究的目的:

合成和描述一系列非循环,单体四二二基酸盐.
为了调查不寻常的结构特征,特别是连接键之间的结合角度.
阐明控制这些几何形状的电子和硬质因素.

主要方法:

合成M(ChAr) 2化合物 (M = Si,Ge,Sn,Pb;Ch = O,S,Se;Ar = m-terphenyl).这些化合物中,M= Si,Ge,Sn,Pb,Ch=O,S,Se,Ar=m-terphenyl) 是最常见的一种.
光谱表征 (NMR,UV-Vis,等等) 的方法 ) 的情况.
单晶X射线衍射用于结构确定.
高级密度函数理论 (DFT) 计算,包括分散校正.

主要成果:

成功合成了一系列广泛的四二二甲基酸盐,包括新的非循环烯.
观察急性联结体,Ch-M-Ch,结合角度,通常低于90°.
连接体大小和连接体间角之间的反向关系:随着连接体大,角度会减少.
DFT计算证实了分散力在稳定这些尖角度方面的重要作用.

结论:

二二基酸盐表现出独特的几何形状,其驱动因素超出了简单的固体排斥.
在这些系统中,分散力对于稳定急性联结结合角度至关重要.
这些发现挑战了对有机金属化合物的固体效应的传统理解.

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