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Plasma-Assisted Chain Reactions of Rh3+ Clusters with Dinitrogen: N≡N Bond Dissociation.

Dinitrogen activation is known as one of the most challenging subjects in chemistry. A number of well-defined metal complexes, nitrides and clusters have been studied showing catalysis for dinitrogen activation. However, direct evidence of a complete cleavage of the N≡N triple bond at mild conditions is rather limited so far. Herein, we report a study on the dissociation of N2 on small rhodium clusters assisted by surface plasma radiation. From mass spectrometry observation, a few rhodium nitride clusters with odd number of nitrogen atoms are produced, such as Rh3N2n-1+ (n=1-5) series, indica-tive of N≡N bond dissociation in the mild plasma atmosphere. Interestingly, Rh3N7+ is identified with outstanding mass abundance among the RhnN2n-1+ products, and its ground-state structure is in the form of Rh3N(N2)3+ by capping a nitrogen atom on the top of Rh3+ plane and hanging three N2 molecules beneath the three Rh atoms respectively, giving rise to a C3v symmetry and excellent stability. We demonstrate the catalysis of such a three-atom rhodium cluster, and reveal a dini-trogen activation strategy by thermodynamics- and dynamics- favorable chain reactions of multiple N2 molecules with two rhodium clusters under plasma atmosphere.