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選択硫化反応を用いる使用済核燃料再処理法

Spent fuel reprocessing process by selective sulfurization

佐藤 修彰*; 佐藤 宗一

Sato, Nobuaki*; Sato, Soichi

使用済燃料から核燃料物質を回収するために、硫化法を用いた方法について試験を行った。本法を用いることにより、(1)低温での硫化反応(2)核分裂生成物のみの硫化(3)核燃料物質は酸化物として回収できることが上げられる。ウラン酸化物と希土類酸化物について二硫化炭素を用いた硫化試験を行いXRD及び熱力学的な観点から評価した。またPuO$$_{2}$$の代替物質としてCeO$$_{2}$$を用いた試験を行った。これらの結果、(1)ボロキシデーションにおいて、U$$_{3}$$O$$_{8}$$が生成し、希土類を固溶した部分はUO$$_{2}$$であること。(2)希土類は選択的に硫化されること。(3)CeO$$_{2}$$はUO$$_{2}$$と似た挙動をとること。(4)硫化された希土類は選択的に溶解されること。(5)Cs, Sr,白金族についても熱力学的な観点から考察した。(6)これらの結果から選択硫化法を用いた核燃料物質の酸化物回収方法について提案した。

For the recovery of nuclear materials from spent oxide fuel, a selective sulfurization method was examined. Sulfurization behavior of uranium and fission products such as rare-earths, was investigated by XRD analysis as well as thermodynamic consideration. The sulfurization behavior of PuO$$_{2}$$ was also investigated by using CeO$$_{2}$$ as a stand-in of PuO$$_{2}$$. The results are summarized as follows; (1)At voloxidation, a part of U$$_{3}$$O$$_{8}$$ changed to rare-earth doped UO$$_{2}$$ solid solution in the presence of rare-earths. (2)Rare-earth oxides were selectively sulfurized, while U$$_{3}$$O$$_{8}$$ was reduced to UO$$_{2}$$. (3)CeO$$_{2}$$ showed a similar sulfurization behavior to that of UO$$_{2}$$. (4)The sulfurized rare-earths selectively dissolved into nitric acid, while UO$$_{2}$$ did not. (5)Sulfurization behaviors of other fission products such as Cs, Sr and platinum group were discussed by thermodynamic consideration. (6)Process for recycling nuclear materials as oxides by selective sulfurization was proposed.

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