Candidate waste forms for immobilisation of waste chloride salt from pyroprocessing of spent nuclear fuel

Candidate waste forms for immobilisation of waste chloride salt from pyroprocessing of spent nuclear fuel
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用于固定乏核燃料高温处理废氯化盐的候选废物形式

DOI:
10.1016/j.jnucmat.2011.09.020
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发表时间:
2012
影响因子:
3.1
通讯作者:
Vance E
Vance E
中科院分区:
工程技术2区
文献类型:
--
作者:
Vance E

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在850°C/100 MPa下热等静压(HIP)制备的方钠石/玻璃体是固定含裂变产物的KCl-LiCl高温处理废盐的候选材料。为了研究方钠石在结构上结合这种高温处理盐的能力,将K、Li、Cs、Sr、Ba和La单独靶向在方钠石中的Na位点中进行取代(Na空位靶向作为碱金属和稀土的电荷补偿剂),并在800-1000°C范围内烧结后通过X射线衍射和扫描电子显微镜进行研究。K和Li似乎进入方钠石,但Cs,Sr和Ba形成铝硅酸盐相和La形成氧磷灰石相。然而,这些非方钠石相对水浸出具有合理的抗性。纯氯磷灰石对方钠石具有上级抗浸出性,并且通常已知碱金属、碱金属和稀土离子会进入氯磷灰石,但是基于扫描电子显微镜,将模拟废盐制剂掺入HIP处理的氯磷灰石基制剂中或将Cs单独取代到Ca基氯磷灰石的结构中的尝试没有成功。材料表现出严重的水溶性,主要是在Cs的释放。试图将Cs替换为Ba和Sr基氯磷灰石的尝试看起来也不令人鼓舞。因此,单独使用磷灰石来保留来自电解核燃料后处理的含有裂变产物的废高温处理盐是有问题的,但氯磷灰石玻璃陶瓷可能是可行的,尽管减少了废物负荷。锂辉石,Ca 2(PO 4)Cl,似乎不适合纳入含氯废物裂变产物。
Sodalite/glass bodies prepared by hot isostatic pressing (HIPing) at ∼850°C/100MPa are candidates for immobilising fission product-bearing waste KCl–LiCl pyroprocessing salts. To study the capacity of sodalite to structurally incorporate such pyroprocessing salts, K, Li, Cs, Sr, Ba and La were individually targeted for substitution in a Na site in sodalite (Na vacancies targeted as charge compensators for alkaline and rare earths) and studied by X-ray diffraction and scanning electron microscopy after sintering in the range of 800–1000°C. K and Li appeared to enter the sodalite, but Cs, Sr and Ba formed aluminosilicate phases and La formed an oxyapatite phase. However these non-sodalite phases have reasonable resistance to water leaching. Pure chlorapatite gives superior leach resistance to sodalite, and alkalis, alkaline and rare earth ions are generally known to enter chlorapatite, but attempts to incorporate simulated waste salt formulations into HIPed chlorapatite-based preparations or to substitute Cs alone into the structure of Ca-based chlorapatite were not successful on the basis of scanning electron microscopy. The materials exhibited severe water leachability, mainly in regard to Cs release. Attempts to substitute Cs into Ba- and Sr-based chlorapatites also did not look encouraging. Consequently the use of apatite alone to retain fission product-bearing waste pyroprocessing salts from electrolytic nuclear fuel reprocessing is problematical, but chlorapatite glass–ceramics may be feasible, albeit with reduced waste loadings. Spodiosite, Ca2(PO4)Cl, does not appear to be suitable for incorporation of Cl-bearing waste containing fission products.
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