The effect of air on oxidation decomposition of uranium-containing cationic exchange resins in Li2CO3-Na2CO3-K2CO3 molten-salt system

RSC Adv. 2023 Jun 19;13(27):18347-18362. doi: 10.1039/d3ra02723f. eCollection 2023 Jun 15.

Abstract

With the development of nuclear energy, spent cationic exchange resins after purification of radioactive wastewater must be treated. Molten-salt oxidation (MSO) can minimize the disposal content of resins and capture SO2. In this work, the decomposition of uranium-containing resins in carbonate molten salt in N2 and air atmospheres was investigated. Compared to N2 atmosphere, the content of SO2 released from the decomposition of resins was relatively low at 386-454 °C in an air atmosphere. The SEM morphology indicated that the presence of air facilitated the decomposition of the resin cross-linked structure. The decomposition efficiency of resins in an air atmosphere was 82.6% at 800 °C. The XRD analysis revealed that uranium compounds had the reaction paths of UO3 → UO2.92 → U3O8 and UO3 → K2U2O7 → K2UO4 in the carbonate melt, and sulfur elements in resins were fixed in the form of K3Na(SO4)2. The XPS result illustrated that peroxide and superoxide ions accelerated the conversion of sulfone sulfur to thiophene sulfur and further oxidized to CO2 and SO2. Besides, the ion bond formed by uranyl ions on the sulfonic acid group was decomposed at high temperature. Finally, the decomposition of uranium-containing resins in the carbonate melt in an air atmosphere was explained. This study provided more theoretical guidance and technical support for the industrial treatment of uranium-containing resins.