Transition metal-catalyzed chemoselective silylation of functionalized terminal alkenes

ORGN 311

Shinji Nakamura, Masanobu Uchiyama, uchiyama@mol.f.u-tokyo.ac.jp, and Tomohiko Ohwada, ohwada@mol.f.u-tokyo.ac.jp. Graduate School of Pharmaceutical Sciences, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo, Japan
While silylmetalation is a versatile method to prepare organosilicon compounds, reactions of inactivated olefins as substrates have been unsuccessful. Recently we have revealed that the dianion-type silylzincate complexes promote highly chemoselective silylzincation of terminal alkynes in the absence of any transition metal catalysts. In our study of scope and limitation of this silylzincation, we found that two kinds of products can be obtained from terminal alkenes, and varying the transition metal catalysts can control the selectivity of the product. Namely, in the presence of copper cyanide, the silylation occurs at the terminal carbon atom selectively and the resultant alkyl zinc intermediates can be trapped by various electrophiles such as deuterium oxide, ally halide, and propargyl halide to give alkylsilanes. On the other hand, in the case of titanocene dichloride, the silylation also occurs regiospecifically at the terminal carbon atom, and subsequent regioselective hydride elimination can occur spontaneously, which gives allylsilanes.