Redox-enabled cooperative catalysis by activating secondary alcohols using low-valent Zn complexes.

Inspired by nature's redox management in bioinorganic systems, we developed various Zn-complexes to catalyze a radical-mediated borrowing hydrogen process for producing β-disubstituted ketones. A diverse range of secondary alcohols, including fatty alcohols, terpenoids and steroid analogs, were successfully utilized for the chemoselective functionalization of ketones. Several organometallic and control studies suggest that coordinatively unsaturated radical species operate as active catalysts to promote alcohol activation and initiate the HAT process.