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In this work, a novel and simple catalytic system including FeCl2, PPh3 and potassium tert-butoxide has been employed for the synthesis of imines from amines. In order to prove the catalytic acceptorless dehydrogenation pathway for this transformation, the liberated H2 gas is detected by NMR spectroscopy. By utilizing this protocol, a variety of arylamines were used successfully for the preparation of corresponding imines in good to excellent yields (on a 1 mmol scale, 73–91% yield for homocoupling, 71 and 91% for heterocoupling). [ABSTRACT FROM AUTHOR]