An efficient, one-pot approach has been established for synthesizing a wide range of 3-amino-[1,2,4]-triazolo pyridines and related heterocycles from the electrochemically induced desulfurative cyclization of 2-hydrazinopyridines with isothiocyanates. The protocol allows for the formation of C−N bonds under simple conditions without transition metals or external oxidants. The practicability of this strategy is demonstrated by its broad substrate scope, good functional group compatibility, and gramscale synthesis. The late-stage modification of 3-amino-[1,2,4]triazolo pyridines enables us to obtain several molecules with potent anticancer activity.

An efficient anodic C­(sp3)–H acyloxylation protocol has been established via intermolecular cross-dehydrogenative C­(sp3)–O coupling. The protocol provides various C2-acyloxy indolin-3-ones without the addition of metal catalysts and external oxidants because indolin-3-ones can be directly oxidized at the anode. The effective application of several medical drugs and the realization of the gram-scale experiment have proven the practicality of this protocol.