Cooperative Triple Catalysis Enables Deaminative α-Indolmethylation of Carbonyl Compounds with Gramines

α-Functionalization of carbonyl compounds is an important reaction in synthetic chemistry. However, the development of novel synthetic strategies to realize this reaction is challenging. This study describes the α-indolmethylation of carbonyl compounds using cooperative copper, amine, and hydrogen-bond catalysis. This reaction provides a novel and efficient strategy for developing indolmethylated carbonyl compounds by deaminative coupling of gramines.