Various Li1-z(Ni1-yFey)(1+z)O-2 materials (0<y<less than or equal to>1) wer
e prepared and characterized by XRD. Phases with a quasi-lamellar O3 type s
tructure are obtained only for y less than or equal to0.30. In order to pre
cisely determine the cationic distribution in the layered phases, a combine
d analysis by X-ray and neutron diffraction, magnetic measurements and also
Mossbauer spectroscopy was performed. The Rietveld refinement of the XRD p
atterns shows that a significant amount of 3d cation is always present in t
he lithium site leading to the formation of ferrimagnetic clusters. A compa
rative Fe-57 Mossbauer study of iron substituted lithium and sodium nickela
te showed that the quadrupolar splittings are very sensitive to the nature
of the iron site. For the largest y and z values iron ions are simultaneous
ly present in the slab and in the interslab space.