The crystalline trilithium salt Li3 [N3N](N3N=[(Me3SiNCH2CH2) 3NI2-) reacts with VCld (DME)(DME= 1, 2-dimethoxyethane) to give [N3N] VCl in 45% yield. The structure of [N3N] VCl, as determined by X-ray crystallography, is a distorted trigonal bipyramid with three equatorial silylamido groups and axial chloride and amine donor ligands. Reduction of [N3N] VCl with Na/Hg in pentane provides trigonal monopyramidal V [N3N] in> 90% yield. ...