ZnO enhanced molten Na2CO3-K2CO3 system for simulated waste resins treatment: Efficient conversion and fixation of organic sulfur and iron(III)

Abstract

The radioactive spent resins from pressurized water nuclear power plant always contain a significant proportion of 55Fe, which invariably leads to the release of radionuclides and acidic gases if not treated promptly. Herein, an efficient ZnO enhanced molten salt oxidation (MSO) method was established for the removal and fixation of organic sulfur and Fe in simulated radioactive resins containing Fe3+ (Fe-CERs). The existence of Fe3+ facilitates the reaction with O2 to form Fe2O3, which contributes to the fracture of organic skeleton. The comparative study was conducted to explore the impact of ZnO on the oxidation behavior of Fe and S at 600–800 °C. The introduction of ZnO caused the continuous formation of ZnS at 600–700 °C, and the conversion of ZnO at 800 °C indirectly promotes the retention rate of S (85.42 %). The potential conversion of Zn0.73Fe0.27S to ZnS may occur within the temperature range of 700 °C to 800 °C. Additionally, the predominant presence of carbon in residues at approximately 700 °C could exert a stimulating effect on the sulfidation process of Fe2O3 and inhibit the formation of SO2. The coexistence of Fe2O3, carbon and ZnO effectively diminishes H2S and SO2 amounts while further enhancing the fixation of S and Fe. The increase generation of K2SO4, FeS and Fe3O4 leads to a high formation rate of SO42- (79.36 %) and a great retention efficiency of Fe (96.23 %) at 800 °C. The proposed novel MSO method holds promising potential for applications in the treatment of organic contaminants.