Electrochemically driven Nickel-Catalyzed Enantioselective Reductive Conjugate (Hetero)Arylation of Enones

03 April 2024, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

Herein, we report an electrochemical nickel-catalyzed enantioselective reductive conjugate (hetero)arylation of enones in an undivided cell with low-cost electrodes in the absence of external reductants. Aryl bromides/iodides/triflates or vinyl bromides were employed as electrophilic reagents for the efficient preparation of more than 50 valuable β-arylated ketones in a simple manner (up to 97% yield, 97% ee). With the advantages of electrochemistry, excellent functional group tolerance and late-stage modification of complex natural products and pharmaceuticals made the established protocol greener and more economic. Mechanism investigation suggest that a NiI/NiIII cycle is involved in this electro-reductive reaction rather than metal reductant driven Ni0/NiII cycle. Overall, the efficient electrochemical activation and turnover of the nickel catalyst avoid the drawbacks posed by the employment of stoichiometric amount of sensitive metal powder reductants.

Keywords

organic electrochemistry
nickel catalysis
enantioselective conjugate arylation
electroreduction
asymmetric electrosynthesis

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