Abstract
Base metal-catalyzed oxidative conversion of ammonia into dinitrogen is a promising process to utilize ammonia as an energy carrier. In this study, we report the manganese-catalyzed ammonia oxidation under chemical and electrochemical conditions. Mechanistic studies including density functional theory (DFT) calculations suggest that a nucleophilic attack of ammonia on manganese nitrogenous complexes occurs to form a nitrogen–nitrogen bond leading to dinitrogen.