Cascade Electrosynthesis of Aryl Imides and Sulfonimides From N₂ via Integrated Nitrogen Fixation and C─N/S─N Bond...

Direct synthesis of organonitrogen compounds from dinitrogen (N₂) remains a formidable challenge because N₂-to-C─N bond formation requires nitrogen fixation to be coupled with selective functionalization of N₂-derived intermediates before their termination as ammonia. Herein, we report a cascade electrochemical strategy that converts N₂ into aryl imides and aryl sulfonimides in a gas-diffusion electrochemical flow cell. Under proton-donor-free conditions, electrochemically generated Li₃N is intercepted by acyl or sulfonyl chlorides, enabling one-pot synthesis of aryl imides and sulfonimides from N₂ in yields up to 57%. This represents a notably high yield for direct N₂-derived organonitrogen synthesis. This work couples N₂ fixation and C─N/S─N bond formation, expanding electrochemical nitrogen fixation beyond ammonia synthesis toward direct construction of value-added C─N/S─N bonds.