The Sequential Activation Of H-2 And N-2 Mediated By The Gas-Phase Sc3n+ Clusters: Formation Of Amido Unit

The activation and hydrogenation of nitrogen are central in industry and in nature. Through a combination of mass spectrometry and quantum chemical calculations, this work reports an interesting result that scandium nitride cations Sc3N+ can activate sequentially H-2 and N-2, and an amido unit (NH2) is formed based on density functional theory calculations, which is one of the inevitable intermediates in the N-2 reduction reactions. If the activation step is reversed, i.e., sequential activation of first N-2 and then H-2, the reactivity decreases dramatically. An association mechanism, prevalent in some homogeneous catalysis and enzymatic mechanisms, is adopted in these gas-phase H-2 and N-2 activation reactions mediated by Sc3N+ cations. The mechanistic insights are important to understand the mechanism of the conversion of H-2 and N-2 to NH3 synthesis under ambient conditions.