Kawano Yasuro, Yamaguchi Kazunori, Miyake Shun-ya, Kakizawa Taeko, Shimoi Mamoru
Department of Basic Science, Graduate School of Arts and Sciences, University of Tokyo, Meguro-ku, Tokyo 153-8902, Japan.
Chemistry. 2007;13(24):6920-31. doi: 10.1002/chem.200601883.
We investigated the influence of a substituent and a Lewis base on boron upon the thermodynamic stability of metal complexes of borane-Lewis base adducts, [M(CO)5(eta1-BH(2)R.L)] (M=Cr, W) and [CpMn(CO)2(eta1-BH2R.L)], where R=Cl, I, m-C6H4F, Ph, H, Me, Et; L=PMe3, PPh3, NMe3, quinuclidine. In these compounds, the stability of the metal-borane linkage was enhanced by increasing the electron-releasing ability of the substituent on boron. A stronger base L additionally stabilized the complexes. The strength of the borane-metal interaction is thus mainly ascribed to the electron donation from the BH sigma orbital to metal rather than the back-donation into the BH sigma* orbital. This result supports the bonding model for the B-H-M linkage in the borane complexes suggested by MO calculations, where the borane-to-metal electron donation is predominant while the metal back-donation into the BH sigma* orbital is negligible. Such a stability trend of the borane complexes makes a sharp contrast to that of many silane and dihydrogen complexes.
我们研究了硼上的取代基和路易斯碱对硼烷 - 路易斯碱加合物的金属配合物热力学稳定性的影响,这些配合物包括[M(CO)5(η1 - BH(2)R·L)](M = Cr、W)和[CpMn(CO)2(η1 - BH2R·L)],其中R = Cl、I、间 - C6H4F、Ph、H、Me、Et;L = PMe3、PPh3、NMe3、奎宁环。在这些化合物中,硼上取代基的给电子能力增强会提高金属 - 硼键的稳定性。更强的碱L会进一步稳定这些配合物。因此,硼烷 - 金属相互作用的强度主要归因于从BHσ轨道向金属的电子给予,而非向BHσ轨道的反馈电子。这一结果支持了分子轨道计算所提出的硼烷配合物中B - H - M键合模型,其中硼烷向金属的电子给予占主导,而金属向BHσ轨道的反馈电子可忽略不计。硼烷配合物的这种稳定性趋势与许多硅烷和二氢配合物的稳定性趋势形成了鲜明对比。