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Chlorination of UO$$_{2}$$ and (U,Zr)O$$_{2}$$ solid solution using MoCl$$_{5}$$

MoCl$$_{5}$$を用いたUO$$_{2}$$及び(U,Zr)O$$_{2}$$固溶体の塩素化

佐藤 匠; 柴田 裕樹; 林 博和; 高野 公秀 ; 倉田 正輝

Sato, Takumi; Shibata, Hiroki; Hayashi, Hirokazu; Takano, Masahide; Kurata, Masaki

東京電力福島第一原子力発電所事故で発生した燃料デブリの処理に乾式処理技術を適応させるための前処理技術の候補として、塩素化力の強いMoCl$$_{5}$$を用いてUO$$_{2}$$及び(U,Zr)O$$_{2}$$模擬デブリを塩化物に転換するための試験条件及び反応副生成物を蒸留分離する条件を調べた。粉末状のUO$$_{2}$$及び(U,Zr)O$$_{2}$$は300$$^{circ}$$Cでほぼ全量が塩化物に転換された。(U,Zr)O$$_{2}$$高密度焼結体については、300$$^{circ}$$Cと400$$^{circ}$$Cでは試料表面のみが塩化物に転換され内部まで反応が進行しなかったが、500$$^{circ}$$Cでは生成したUCl$$_{4}$$が蒸発して試料表面から分離されたためにほぼ全量が塩化物に転換された。反応副生成物であるMo-O-Clは、温度勾配下での加熱によりUCl$$_{4}$$から蒸留分離された。

In order to explore the applicability of the chlorination by MoCl$$_{5}$$ as a potential pretreatment technique for waste treatment of fuel debris by pyrochemical methods, chlorination experiments of UO$$_{2}$$ and (U$$_{0.5}$$Zr$$_{0.5}$$)O$$_{2}$$ simulated fuel debris were carried out in two steps: the first one is a chlorination reaction by homogeneous heating, the second one is a volatilization of molybdenum by-product by heating under temperature gradient condition. Most of UO$$_{2}$$ and (U$$_{0.5}$$Zr$$_{0.5}$$)O$$_{2}$$ powder were converted to UCl$$_{4}$$ or UCl$$_{4}$$ and ZrCl$$_{4}$$ mixture at 573 K, respectively. In the case of (U$$_{0.5}$$Zr$$_{0.5}$$)O$$_{2}$$sintered particle, most of sample was converted to the chlorides because the products evaporated and be separated from sample surface at 773 K, while only the surface of the sample disk was converted to the chlorides at 573 and 673 K. Most of molybdenum by-product and ZrCl$$_{4}$$ were separated from UCl$$_{4}$$ by volatilization at 573 K.

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パーセンタイル:81.41

分野:Nuclear Science & Technology

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