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First-principles methods are used to calculate the miscibility of eight aluminum-doped transition-metal oxides in the layered α-NaFeO 2 structure. This study finds that for all Li(Al,M)O 2 compounds investigated (M = Ti, V, Cr, Mn, Fe, Co, Ni, Cu) the enthalpy of mixing is positive. In addition, detailed analyses were performed on LiAl 1- xCoxO2 and LiAl 1-x Cr x O 2 by calculating full temperature-composition phase diagrams. For the Li(Al,Co)O 2 system, we find regions of immiscibility below - 173°C and above 600°C. For both Li(Al,Co)O 2 and Li(Al,Cr)O 2 above 600°C, Al-doping is limited by the formation of γ-LiAlO 2 .

Phase Separation Tendencies of Aluminum‐Doped Transition‐Metal Oxides ( LiAl1 − x M x O 2 ) in the α ‐ NaFeO2 Crystal Structure