The sustainable management of spent nuclear fuel (SNF) poses significant challenges, particularly in reducing high-level radioactive waste. To address these issues, high-radiation-generating rare-earth elements (RE), must be converted into stable forms for safe long-term storage in a deep geological repository. This study explores the conversion of RECl3 (RE = Y, La, Ce, Pr, Nd, and Sm) to their corresponding oxides through reactive distillation via a solid–solid reaction with K2CO3. It is crucial for reducing the volume and increasing the safety of geological disposal of nuclear waste. Thermodynamic calculations indicate that the reaction between RECl3 and K2CO3 proceeds favorably without a molten salt, as evidenced by low Gibbs free energy values. Experimentally, the reaction was conducted by mixing RECl3 with K2CO3 in a 1: 2.55 M ratio, followed by heating at 550 °C under 0.9 bar and then at 850 °C under vacuum. X-ray diffraction and scanning electron microscopy analyses results confirm the effective conversion of RECl3 to high-purity RE oxides. Additionally, experiments using a simulated mixture of RECl3, reflecting actual SNF composition, yielded the same results, demonstrating that RE oxides can be produced even in mixtures. It further emphasizes the process's applicability to real-world SNF management. The proposed approach can enhance the process efficiency as this method allows the oxidation of RECl3 and the subsequent separation of byproduct (KCl and CO2) to be performed within one reactor.
扫码关注我们
求助内容:
应助结果提醒方式:
