Various disposal methods for spent nuclear fuels (SNFs) are being researched, and one of these methods involves separating high heat-generating nuclear isotopes such as Strontium-90 (90Sr) and Cesium-137 (137Cs) for deep disposal. These isotopes has relatively short half-lives and substantial decay energies. Especially, 90Sr undergoes decay through Yttrium-90 to Zirconium-90, emitting intense heat with beta radiation. Therefore, the removal of these high heat-generating isotopes will significantly contribute to reducing disposal site area. To remove 90Sr from SNFs, molten salt was utilized in KAERI. During this process, it was discovered that 90Sr dissolves in the molten salt in the form of SrCl2 and/or Sr4OCl6. Afterwards, it is crucial to recover 90Sr in the form of oxide from the salt to create immobilized forms for disposal. This can be achieved by reactive distillation with K2CO3. However, the amount of 90Sr within the SNFs is only 0.121wt%, and even if all the 90Sr in the SNFs were to leach into the molten salt, the quantity of 90Sr in the molten slat would still be very small. Therefore, adding K2CO3 to the molten salt for reactive distillation could result in significant possibilities of side reactions occurring. In this study, a two-step process was employed to mitigate the side reactions: the 1st step involves evaporating the all molten salts and the 2nd step includes adding K2CO3 to make oxides through solid-solid reaction. Eutectic LiCl-KCl, which is the most commonly used salt, was employed. The eutectic LiCl-KCl with SrCl2 was heated at 850°C for 2 h to evaporate the salts under a vacuum (> 0.02 torr). However, after examining the distillation product before the solid-solid reaction, it was observed that SrCl2 reacted with KCl in the salt, resulting in the formation of KSr2Cl5. It means that salts containing KCl are not suitable candidates for reactive distillation aimed at producing immobilized forms. As an alternative, MgCl2 could be a highly promising candidate because it is inert to SrCl2 and according to a recent study in KAERI, MgCl2 exhibited the most efficient separation of Sr among various salts. Therefore, we plan to proceed with the two-step reactive distillation using MgCl2 for the future work.

사용후핵연료 파이로프로세싱에서 발생하는 방사성폐기물의 양을 최소화하기 위해서는 방사성 핵종 함유 염폐기물을 효과 적으로 처리할 수 있는 기술개발이 필요하다. 이를 위해 탄산화물(Li2CO3, K2CO3)을 이용한 반응증류공정에서 LiCl-KCl 공융 염 내 NdCl3의 분리특성을 관찰하였다. HSC-Chemistry 프로그램을 이용한 탄산화물과 NdCl3의 반응모델결과에서 NdCl3는 탄산화물의 주입조건 및 온도변화에 따라 산염화물(NdOCl) 또는 산화물(Nd2O3) 형태로 전환됨이 확인되었으며, 탄산화물 의 주입조건에 따른 LiCl-KCl-NdCl3계의 반응증류시험에서 반응모델결과와 유사한 경향을 확인하였다. 이 결과들을 이용하 여 LiCl-KCl 공융염 내 NdCl3를 고화가 용이한 산화물 형태로 분리하기 위한 공정조건을 도출하였다.