Alkylation of an N2‐Derived PN3P Mo(V) Nitride Complex

Abstract The alkylation of a nitride ligand of a post‐modified Mo(V) complex was achieved with MeOTf ( 1 a ) and EtOTf ( 2 a ), respectively. However, different from the known Mo(VI) nitride complexes where the alkyl group can be deprotonated by strong bases to form a ketimide for the next progressive reactions leading to nitrile, 1 a and 2 a can only be reduced to highly stable Mo(IV) imido complexes by NaH. Upon treatment with fresh PhCH 2 OTf, a new dinuclear Mo complex was isolated with N 2 release, instead of benzylation of the nitride ligand.