Theoretical predictions and single-crystal neutron diffraction and inelastic neutron scattering studies on the reaction of dihydrogen with the dinuclear dinitrogen complex of zirconium [P2N2]Zr(mu-eta2-N2)Zr[P2N2], P2N2 = PhP(CH2SiMe2NSiMe2CH2)2PPh

A study was undertaken to analyze the dinitrogen complex of zirconium [P2N2]Zr(mu-eta2-N2)Zr[P2N2] wherein P2N2 = PhP(CH2SiMe2NSiMe2CH2)2PPh reacted with 1-4 atm of H2 in toluene solution to form the [P2N2]Zr(mu-eta2-N2H)(mu-H)Zr[P2N2] (2) having an N-H bond and a bridging hydride. Results of the neutron studies and density functional theory revealed that the dinuclear dihydrogen complex, [P2N2]Zr(mu-eta2-N2)(mu-eta2-H2)Zr[P2N2], was an artifact of the X-ray analysis while solution 2 was identical to the solid-state structure.