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According to the ion and molecule coexistence theory (IMCT) for molten slags and corresponding phase diagrams, a thermodynamic model for the evaluation of mass action concentrations (designated by Ni for structure unit i) for Ce2O3-Al2O3, CaO-Al2O3-Ce2O3 and CaO-Al2O3-SiO2-Ce2O3 slag systems has been formulated. The results show that when the mole fraction of Ce2O3 is at 0.49 in the binary slag, the mass action concentration of Ce2O3·Al2O3 achieves its maximum value 0.90. In a composition area of CaO/Al2O3 (mass fraction ratio) from 0.7 to 1.5 and Ce2O3 content (mass fraction) from 0 to 45% of the ternary slag at 1773 K, the results show that trends of calculated NAl2O3 are in good agreement with reported measured trends of aAl2O3. The iso-curves of NCe2O3 and NCaO are also drawn from the calculated results. A thermodynamic model of the equilibrium between 55.83%CaO-23%Al2O3-11.17%SiO2-10%Ce2O3 quaternary slag and molten steel containing aluminum has been further discussed. Results indicate that certain content of Ce would be dissolved in steel, which increases with the increasing of temperature and aluminum content, and when the aluminum content is 0.02%, the corresponding cerium content is in the range of 1.87 to 13.30 ppm at 1873 K. In summary, using Ce2O3 to replace Al2O3 can effectively reduce NAl2O3, certain content of Ce can dissolved in steel.