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Experimental Study on the Chemical Separation of Actinides in a Pyrochemical Systems

热化学系统化学分离锕系元素的实验研究

基本信息

批准号：
09480101
负责人：
YAMANA Hajimu
金额：
$ 7.36万
依托单位：
KYOTO UNIVERSITY
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (B)
财政年份：
1997
资助国家：
日本
起止时间：
1997 至 1999
项目状态：
已结题

项目摘要

Two molten salt systems, (1) anhydrous molten chloride and(2)hydrate-melt of calcium nitrate were experimentally studied as optional techniques for the separation of actinides and fission products Thermodynamic properties and chemical systematics of actinides and lanthanides in these systems were mainly studied.(1)Pyrometallurgical separation using molten chloride and liquid metals: In a pyrometallurgical liquid-extraction system, which is usable for dry-reprocessing of spent nuclear fuels, some thermodynamic quantities related to their affinity to the solvent materials were studied. A reductive extraction of f-elements in a system of molten alkaline chloride and liquid Bi and Zn were measured, and the excess free energies of tri-valent f-elements in alkaline molten chloride and liquid metal phase were determined. Their systematic variations along the f-series were studied to elucidate the distribution behaviors.(2)Solvent extraction of f-elements by TBP from hydrate-melt of calcium nitrate: Extraction distributions of actinides and lanthanides between tri-butyl phosphate solution and molten calcium nitrate tetra-hydrate (Ca(NOィイD23ィエD2)ィイD22ィエD2・4HィイD22ィエD2O) were radiochemically studied. The apparent equilibrium constants of the extraction reactions of the lanthanides were determined and their characteristic systematics along the lanthanide series was discussed. Based on the results of the distribution behaviors, the characteristics of the in-perfect hydration of trivalent f-cations in the hydrate-melt were discussed.

实验研究了两种熔盐体系：（1）无水熔融氯化物体系和（2）硝酸钙水合物-熔融体系，作为分离锕系元素和裂变产物的可选技术。（1）使用熔融氯化物和液态金属的火法冶金分离：在可用于乏核燃料干法后处理的火法冶金液体萃取系统中，研究了与溶剂材料亲和力有关的一些热力学量。测定了F元素在熔融碱金属氯化物-液态Bi、Zn体系中的还原萃取，测定了F元素在熔融碱金属氯化物和液态金属相中的过剩自由能。它们的系统变化沿着的f系列进行了研究，以阐明分布行为。（2）TBP从CaNO_3-熔融体系中萃取F ~-元素：用放射化学方法研究了锕系元素和镧系元素在Ca（NO ↓ [2] O ↓ [23] O ↓ [2] D ↓ [2]）↓ [22] O ↓ [23] O ↓ [2] O中的萃取分配。测定了镧系元素萃取反应的表观平衡常数，并讨论了它们沿镧系的沿着特征体系。根据分布行为的结果，讨论了三价氟离子在水合物熔体中的不完全水化特征。