Lewis Base Catalyzed Selective Chlorination of Monosilanes

Chemistry. 2018 Dec 3;24(67):17796-17801. doi: 10.1002/chem.201803921. Epub 2018 Nov 5.

Abstract

A preparatively facile, highly selective synthesis of bifunctional monosilanes R2 SiHCl, RSiHCl2 and RSiH2 Cl is reported. By chlorination of R2 SiH2 and RSiH3 with concentrated HCl/ether solutions, the stepwise introduction of Si-Cl bonds is readily controlled by temperature and reaction time for a broad range of substrates. In a combined experimental and computational study, we establish a new mode of Si-H bond activation assisted by Lewis bases such as ethers, amines, phosphines, and chloride ions. Elucidation of the underlying reaction mechanisms shows that alcohol assistance through hydrogen-bond networks is equally efficient and selective. Remarkably, formation of alkoxysilanes or siloxanes is not observed under moderate reaction conditions.

Keywords: Lewis bases; bifunctional silanes; chlorination; density functional calculations; reaction mechanisms.