Breit Nora C, Szilvási Tibor, Inoue Shigeyoshi
Department of Chemistry, Technische Universität Berlin, Straße des 17. Juni 135, Sekr. C2, 10623 Berlin (Germany), Fax: (+49) 30-314-29732.
Chemistry. 2014 Jul 21;20(30):9312-8. doi: 10.1002/chem.201402693. Epub 2014 Jun 26.
An acyl-functionalized phosphasilene, LSi(COtBu)=P(SiMe3) (L = PhC(NtBu)2) was synthesized on a new route by the addition of tBuCOCl to the phosphinosilylene LSiP(SiMe3)2 and subsequent Me3SiCl elimination. DFT studies elucidated its molecular structure, the influence of the acyl group on UV/Vis transitions, and revealed the mechanism. The intermediate LSi(COtBu)ClP(SiMe3)2, with a five-coordinate silicon center, was characterized by NMR spectroscopy and X-ray analysis. On the other hand, phosphasilene LSi(SiMe3)=P(SiMe3) reacted with tBuCOCl by a [2+2] cycloaddition of the silicon-phosphorus double bond and the carbon-oxygen double bond in addition to Me3SiCl elimination, thereby affording the novel, fully characterized compound LSi(SiMe3)[P=C(tBu)O] bearing a Si-P-C-O heterocycle with a phosphorus-carbon double bond. DFT studies suggest that two mechanisms occur simultaneously.
通过将叔丁基甲酰氯添加到膦基硅烯LSiP(SiMe3)2中并随后消除三甲基氯硅烷,在一条新路线上合成了一种酰基官能化的磷硅烯LSi(COtBu)=P(SiMe3)(L = PhC(NtBu)2)。密度泛函理论(DFT)研究阐明了其分子结构、酰基对紫外/可见跃迁的影响,并揭示了反应机理。具有五配位硅中心的中间体LSi(COtBu)ClP(SiMe3)2通过核磁共振光谱和X射线分析进行了表征。另一方面,磷硅烯LSi(SiMe3)=P(SiMe3)除了消除三甲基氯硅烷外,还通过硅-磷双键与碳-氧双键的[2+2]环加成反应与叔丁基甲酰氯反应,从而得到了具有磷-碳双键的含Si-P-C-O杂环的新型、完全表征的化合物LSi(SiMe3)[P=C(tBu)O]。DFT研究表明两种机理同时发生。