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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 O2to 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 Fe2O3and inhibit the formation of SO2. The coexistence of Fe2O3, carbon and ZnO effectively diminishes H2S and SO2amounts while further enhancing the fixation of S and Fe. The increase generation of K2SO4, FeS and Fe3O4leads 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.

ABSTRACTThe oxidation characteristics of anionic exchange resins (AERs) during molten salt oxidation (MSO) were investigated in carbonate melt. The residue after MSO of AERs were carbon, which was confirmed by the X-ray diffraction (XRD) and Raman spectra. The remaining amount of salt-free residue after MSO was evaluated by destruction and removal efficiency (DRE), which indicates that 2 hours is a suitable oxidation time. The morphologies of the AERs after MSO were observed by scanning electron microscopy (SEM). The oxidation process of AERs in MSO was investigated by thermogravimetric analysis (TG) and Fourier Transform Infrared Spectrometer (FT-IR), which revealed that initial AERs, experienced four reaction stages in MSO: dehydration, thermal decomposition of functional groups, carbonization of styrene-divinylbenzene copolymer (ST-DVB), and gasification of carbon. The TG data proved that the presence of carbonate promotes the carbonization process of ST-DVB in AERs. The reason why salt catalyzes this stage had been proved to be that the carbonate captures the nitrogen-containing exhaust gas generated by the oxidation of the anion resin, and produces nitrate with catalytic oxidation ability, which catalyzes the oxidation of the resins effectively. This means that MSO will be an environmentally friendly and efficient method for catalytic oxidation of AERs.

With the continuous development of the nuclear industry, there is an urgent need to find a method that can safely and efficiently dispose of spent resins. Molten salt oxidation (MSO) is a promising waste treatment technology. In this paper, the newly shipped resins were used to simulate the actual spent ion exchange resins. The destruction of the resins is mainly divided into three stages. The addition of oxygen can increase the activation energy (E) required for the reaction. Some solid residues which were proved to be amorphous carbon materials generated after MSO. In the high-resolution XPS spectra of C 1s, the C-S bond disappeared after MSO at 400 ℃ for 2 h proved the destruction of the sulfonic acid groups. The core-level scan XPS spectra of S 2p illustrated that sulfur and sulfonyl bridges were formed after sulfonic acid groups were destroyed. The infrared spectrum also showed that the sulfonic acid groups were destroyed at 400 ℃ to form sulfonyl structure, but sulfur bridges were not found due to its small IR absorptions. In this paper, the ternary eutectic Li2CO3-Na2CO3-K2CO3, can be operated efficiently at a relatively low temperature. The generated sulfur dioxide is captured by the carbonate to form sulfate. These merits make MSO become a promising and environmentally friendly approach for the treatment of sulfur-containing organic waste.