Mutual Functionalization of Dinitrogen and Methane Mediated by Heteronuclear Metal Cluster Anions CoTaC

The direct coupling of dinitrogen (N) and methane (CH) to construct the N-C bond is a fascinating but challenging approach for the energy-saving synthesis of N-containing organic compounds. Herein we identified a likely reaction pathway for N-C coupling from N and CH mediated by heteronuclear metal cluster anions CoTaC , which starts with the dissociative adsorption of N on CoTaC to generate a Ta -N (terminal-nitrogen) Lewis acid-base pair (LABP), followed by the further activation of CH by CoTaCN to construct the N-C bond. The N[triple bond, length as m-dash]N cleavage by CoTaC affording two N atoms with strong charge buffering ability plays a key part, which facilitates the HC-H cleavage the LABP mechanism and the N-C formation a CH migration mechanism. A novel N triggering strategy to couple N and CH molecules using metal clusters was accordingly proposed, which provides a new idea for the direct synthesis of N-containing compounds.