The relative partial molal free energy of gallium and the activity of gallium in the compound NiGa have been obtained across the homogeneity range of this phase at 835° and 900°C. A solid state anion conductor ( CaO ‐ stabilized ZrO 2 ) was used as the electrolyte in a high temperature galvanic cell. It was found that the thermodynamic properties of NiGa change rapidly near 50 atom per cent gallium. A brief review is made of the metal/oxide equilibria and the free energies of the two gallium oxides Ga 2 O 3 and Ga 2 O .