Highly facile approach of chemoselective alkylation of α‐oxo compounds such as α‐keto amides, α‐keto esters, isatins, and cyclic‐α‐diketones is developed through C(sp3)‐H functionalization of 2‐methyl quinolines under solvent and catalyst‐free conditions. Further, we complemented the efficacy of this green synthetic protocol by demonstrating the broad substrate diversity, gram‐scale synthesis, and new synthetic transformations of the obtained products.
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