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Frustrated Lewis Pairs Comprising Nitrogen Lewis Acids for Si–H Bond Activation

Idan Avigdori, Alla Pogoreltsev, Alexander Kaushanski, Natalia Fridman, Mark Gandelman

2020Angewandte Chemie International Edition43 citationsDOI

Abstract

Abstract N‐heterocyclic nitrogen Lewis acids are a recent addition to the field of organic chemistry. Based on nitrenium cations, these acids where previously shown to generate Lewis adducts when combined with the appropriate Lewis bases. Herein, a triazinium‐based Lewis acid was combined with t Bu 3 P to generate a frustrated Lewis pair (FLP) capable of cleaving, for the first time, Si−H bonds in silanes. Whereas low yields were initially encountered owing to insufficient Lewis acidity, a new nitrenium‐based Lewis acid was synthesized, and its superior Lewis acidity was experimentally and computationally confirmed. A FLP based on this acid cleaved the Si−H bond in PhSiH 3 , generating the triazane product in a quantitative yield. This unprecedented N−H triazane was fully characterized by multinuclear NMR techniques and single‐crystal X‐ray crystallography. A new class of compounds, N‐H triazanes display the potential capacity to participate in hydride transfer reactions.

Topics & Concepts

Lewis acids and basesChemistryFrustrated Lewis pairAdductNitrogenBoranesYield (engineering)SilanesMedicinal chemistryPolymer chemistryStereochemistryOrganic chemistryBoronCatalysisSilaneMaterials scienceMetallurgyOrganoboron and organosilicon chemistryCatalytic Cross-Coupling ReactionsN-Heterocyclic Carbenes in Organic and Inorganic Chemistry
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