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Base-Modulated 1,3-Regio- and Stereoselective Carboboration of Cyclohexenes

Click:      Time:11.July 2023

Abstract: While chain-walking stimulates wide interest in both
polymerization and organic synthesis, site- and stereoselective
control of chain-walking on rings is still a challenging task in the realm
of organometallic catalysis. Inspired by a controllable chain-walking
on cyclohexane rings in olefin polymerization, we have developed a
set of chain-walking carboborations of cyclcohexenes based on nickel
catalysis. Different from the 1,4-
trans-selectivity disclosed in polymer
science, a high level of 1,3-regio- and
cis-stereoselectivity is obtained
in our reactions. Mechanistically, we discovery that the base affects
the reduction ability of B
2pin2 and different bases lead to different
catalytic cycles and different regioselective products (1,2- Vs 1,3-
addition). This study provides a concise and modular method for the
synthesis of 1,3-disubstituted cyclohexylboron compounds. The
incorporation of a readily modifiable boronate group greatly enhances
the value of this method, the synthetic potential of which was
highlighted by the synthesis of a series of high-valued commercial
chemicals and pharmaceutically interesting molecules.

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