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A novel type of transition bimetal–organic frameworks was described as a heterogeneous catalyst for the oxidative coupling of amines to imines under mild conditions, which was easily synthesized by the coordination assembly of manganese(II) and cobalt(II) with 1,3,5-benzenetricarboxylic acid (H3BTC) for the first time. The metal–organic framework material was characterized by scanning electron microscopy, energy dispersive spectroscopy, X-ray photoelectron spectroscopy, X-ray diffraction, thermogravimetry and N2 sorption. As an environmentally benign heterogeneous catalyst, the catalytic ability of the metal–organic framework material was then detected to be excellent for the tert-butyl hydroperoxide (TBHP) promoted direct oxidative coupling of benzylamines to imines in excellent yields (up to 100%) in methanol for 3 h. More importantly, it could be recycled up to six runs, while still maintaining its high catalytic activity.

Plentiful tertiary amine derivates are synthesized by direct formation of tertiary amines by the interaction of aldehydes with secondary amines over Pt nanowires under mild conditions. This method offers a green and rapid approach to transform secondary amines into various tertiary amines.