Directly transformation of N2 into organophosphine molecules provides a novel and attractive route to these important N-containing compounds. Herein, a synthetic cycle for iminophosphorane synthesis was described. By the addition of iodine and phosphine (PR3), N=P bond was straightforwardly formed on the N2-derived molybdenum terminal nitride featuring a pincer ligand. Subsequent PCET under CO liberated the protonated iminophosphorane, accompanied with the formation of molybdenum tricarbonyl complex. Finally, photo induced oxidative decarbonylation followed by reduction under N2 revived the dimeric N2 bridged complex. Key intermediates were isolated and characterized. The method was applicable for both aryl and alkyl substituted phosphines, offering new ideas for the utilization of N2 beyond ammonia under mild conditions.

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