Cu‐UiO‐66 Catalyzed Synthesis of Imines via Acceptorless Dehydrogenative Coupling of Alcohols and Amines

Herein, the Cu-UiO-66 catalyst was developed for acceptorless dehydrogenative coupling (ADC) between alcohols and amines to produce imines. The Cu-UiO-66 catalyst was synthesized by installing Cu²⁺ onto Zr-oxo clusters in UiO-66, and the catalyst efficiently catalyzes the ADC reaction under mild and environmentally friendly conditions with excellent selectivity. Mechanistic studies reveal that the O₂⋅^- radicals and porosity of formed in Cu-UiO-66 participate cooperatively during the catalytic cycle. Meanwhile, the only by-product of the system is environmentally benign water. Cycling tests and hot filtration tests showed that the Cu-UiO-66 catalyst exhibited excellent stability and catalytic activity during the reaction. Importantly, the Cu-UiO-66 catalyst might provide a promising strategy for the ADC reaction between alcohols and amines to produce imines.