Kabi, Arup K.Gujjarappa, RaghuramRoy, AnupamSahoo, AbhishekMusib, DulalVodnala, NagarajuSingh, VirenderMalakar, Chandi C.2024-01-212024-08-132024-01-212024-08-132021-10-1922326310.1021/acs.joc.1c01450http://10.2.3.109/handle/32116/3223This report describes an efficient transition-metal-free process toward the transfer hydrogenative cascade reaction between nitroarenes and amines or alcohols. The developed redox-economical approach was realized using a combination of KOtBu and Et3SiH as reagents, which allows the synthesis of benzimidazole derivatives via ?-bond metathesis. The reaction conditions hold well over a wide range of substrates embedded with diverse functional groups to deliver the desired products in good to excellent yields. The mechanistic proposal has been depicted on the basis of a series of control experiments, mass spectroscopic evidence which is well supported by density functional theory (DFT) calculations with a feasible energy profile. � 2021 American Chemical Society.en-USAminesDensity functional theoryBenzimidazole derivativesBenzimidazolesCascade reactionsControl experimentsMechanisticsMetal freeNitroarenesReaction conditionsSpectroscopic evidence?-bond metathesisTransition metalsArticlehttps://pubs.acs.org/doi/10.1021/acs.joc.1c01450