The Li2CO3–Na2CO3–K2CO3 carbonate system exhibits superior sulfur interception capacity and thermodynamic stability in the molten salt oxidation (MSO) of cation exchange resins (CERs) with high sulfur content. However, the spent salt from the MSO process cannot be reused to reduce the operating cost and further improve the reduction ratio. Therefore, the optimal oxygen equivalent for treatment is obtained by thermodynamic equilibrium analysis of the MSO process of CERs as 1.08 multiples of the theoretical oxygen demand and the corresponding approximate chemical formula in this work. The results of the equilibrium analysis are used as the basis to propose a replenishment cycle for the MSO process (MSO-RC), which replenishes the consumed carbonate to restore the SO2 adsorption capacity and treatment capacity of the spent salt. During the experiments, the oxidation efficiencies of MSO-RC are higher than 99%, and the volume reduction ratio is improved by 12% compared with the traditional MSO. In addition, the MSO-RC maintains sulfur interception rates above 80% across multiple cycles and preserves over 94.7% Li2CO3 by adding cost-effective Na2CO3 and K2CO3 into the molten salt system. The MSO-RC process significantly improves the efficiency of process operation with lower operational costs.
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