The merging of transition metal catalysis with electrochemistry has become a powerful tool for organic synthesis because catalysts can govern the reactivity and selectivity.However,coupling catalysts with alkyl radica...The merging of transition metal catalysis with electrochemistry has become a powerful tool for organic synthesis because catalysts can govern the reactivity and selectivity.However,coupling catalysts with alkyl radical species generated by anodic oxidation remains challenging because of electrode passivation,dimerization,and overoxidation.In this study,we developed convergent paired electrolysis for the coupling of nickel catalysts with alkyl radicals derived from photoinduced ligand-to-metal charge-transfer of cyclic alcohols and iron catalysts,providing a practical method for site-specific and remote arylation of ketones.The synergistic use of photocatalysis with convergent paired electrolysis can provide alternative avenues for metal-catalyzed radical coupling reactions.展开更多
基金supported by the National Key R&D Program of China(2021YFA1500100)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB0610000)+2 种基金the National Natural Science Foundation of China(21821002,22361142834,and 22101294)the S&TCSM of Shanghai(21ZR1476500)Natural Science Foundation of Ningbo(2023J035)。
文摘The merging of transition metal catalysis with electrochemistry has become a powerful tool for organic synthesis because catalysts can govern the reactivity and selectivity.However,coupling catalysts with alkyl radical species generated by anodic oxidation remains challenging because of electrode passivation,dimerization,and overoxidation.In this study,we developed convergent paired electrolysis for the coupling of nickel catalysts with alkyl radicals derived from photoinduced ligand-to-metal charge-transfer of cyclic alcohols and iron catalysts,providing a practical method for site-specific and remote arylation of ketones.The synergistic use of photocatalysis with convergent paired electrolysis can provide alternative avenues for metal-catalyzed radical coupling reactions.
