There is a high iron content in nickel slag that mainly exists in the fayalite phase. Basic oxide can destroy the stable structure of fayalite which is beneficial to the treatment and comprehensive utilization of nickel slag. The research was based on the composition of the raw nickel slag, taking the CaO-SiO₂-FeO-MgO system as the object and CaO as a modifier. The effect of basicity on the melting characteristics, viscosity and structure of the CaO-SiO₂-FeO-MgO system was studied. The relationship between the viscosity and structure of the CaO-SiO₂-FeO-MgO system was also explored. The results show as follows: (1) When the basicity is lower than 0.90, the primary phase of the slag system is olivine phase. When the basicity is greater than 0.90, the primary phase of the slag system transforms into monoxide. When the basicity is 0.90, olivine and monoxide precipitate together as the temperature continues to decrease. At the same time, the liquidus temperature, softening temperature, hemispherical temperature, and flow temperature all reach the lowest value. (2) With the increase of basicity, the critical viscosity temperature of the CaO-SiO₂-FeO-MgO system decreases first and then increases. Critical viscosity temperature is the lowest at the basicity of 0.90, which is 1295 °C. (3) When the slag system is heterogeneous, the viscosity of the molten slag increases rapidly because of the quantity of solid phase precipitated from the CaO-SiO₂-FeO-MgO system. (4) When the slag system is in a homogeneous liquid phase, the molar fraction of O⁰ decreases with the increase of basicity and the mole fraction of O^-, and O^2- increases continuously at the basicity of 0.38~1.50. The silicate network structure is gradually depolymerized into simple monomers, resulting in the degree of polymerization, and the viscosity, being reduced. The mole fraction of different kinds of oxygen atoms is converged to a constant value when the basicity is above 1.20.

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