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To improve the efficacy of molecular syntheses, researchers wish to capitalize upon the selective modification of otherwise inert C–H bonds. The past two decades have witnessed considerable advances in coordination chemistry that have set the stage for transformative tools for C–H functionalizations. Particularly, oxidative C–H/C–H and C–H/Het–H transformations have gained major attention because they avoid all elements of substrate prefunctionalization. Despite considerable advances, oxidative C–H activations have been dominated by precious transition metal catalysts based on palladium, ruthenium, iridium, and rhodium, thus compromising the sustainable nature of the overall C–H activation approach. The same holds true for the predominant use of stoichiometric chemical oxidants for the regeneration of the active catalyst, prominently featuring hypervalent iodine(III), copper(II), and silver(I …