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The first thermally stable, neutral, electrophilic phosphinidene complexes of vanadium, [CpV(CO)3{\u3b71-P(NR2)}] (R = iPr (3a), Cy (3b)), have been prepared by the reaction of [Na]2[CpV(CO)3] with Cl2PNR2. The molecules 3a and 3b have been characterized by microanalysis, IR, and 1H and 31P{1H} NMR spectroscopy, and for 3a also by single-crystal X-ray diffraction. The structure of 3a exhibits a piano stool geometry closely related to that of CpV(CO)4 with an \u3b71-phosphinidene ligand replacing CO in one of the basal coordination sites of the vanadium atom (V(1)\u2212P(1) = 2.300(2) \uc5). The reactivity of 3a toward a variety of unsaturated substrates: PhC\u2261CPh, di-tBu-imidazol-2-ydene, PhN3, and Ph2C\u2550N\u2550N has been examined to probe the electrophilic (or nucleophilic) character of the low-coordinate P(I) site. In all cases reactions occur exclusively at the phosphinidene phosphorus atom, without CO displacement, affording examples of P-coordinated phosphirene [CpV(CO)3{P(NiPr2)CPh\u2550CPh}] (7), abnormal NCN carbene adduct [CpV(CO)3{P(NiPr2)-4-cyclo-C3H2-1,3-(NtBu)2)}] (8), diazaphosphaimine [CpV(CO)3{P(NiPr2)\u2550N\u2212N\u2550CPh2}] (12), and P-coordinated phosphaimine [CpV(CO)3{P(NiPr2)\u2550NPh}] (14) complexes. The \u3b71-phosphaimine complexes 12 and 14 lose carbon monoxide to yield derivatives [CpV(CO)2{P(NiPr2)N\u2212N\u2550CPh2}] (9) and [CpV(CO)2{P(NiPr2)\u2550NPh}] (15), which contain \u3b72-(P,N)-coordinated phosphaimine ligands. An \u3b73-(P,N,N)-bound phosphaimine ligand is present in an isomer of 9, namely, [CpV(CO)2{P(NiPr2)N\u2212N\u2550CPh2}], 13. Complexes 3a, 7, 8, 9, 14, and 15 have been characterized by X-ray crystallography.Peer reviewed: YesNRC publication: Ye

Synthesis and Structural Characterization of the First Thermally Stable, Neutral, and Electrophilic Phosphinidene Complexes of Vanadium