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フルオラスリン酸エステルによるZr(IV)の抽出; リン酸トリブチルとの比較

A Fluorous phosphate for the extraction of Zr(IV) from HNO$$_{3}$$ solution; Comparison with tri-$$n$$-butyl phosphate

上田 祐生 ; 菊池 圭; 杉田 剛  ; 徳永 紘平  ; 元川 竜平  ; 長縄 弘親 

Ueda, Yuki; Kikuchi, Kei; Sugita, Tsuyoshi; Tokunaga, Kohei; Motokawa, Ryuhei; Naganawa, Hirochika

リン酸トリブチル(TBP)を用いた 従来のPUREXプロセスにおいて多量のZr(IV)が含まれる場合、抽出錯体, 遊離の抽出剤, 酸、および水の凝集を起源として生成する不溶性の第三相や沈殿による目的物の抽出阻害が問題であった。本研究では水にほとんど溶解しないフルオラス化合物に着目し、TBPと同一のリン酸エステル構造を有するフルオラスリン酸エステル抽出剤を合成し、本抽出剤のZr(IV)抽出特性、抽出機構、および第三相生成の抑制効果をTBPと比較検証した。開発した新規抽出剤は、TBPと比較し第三相の生成を著しく抑制するとともに、幅広い硝酸濃度領域においてTBPよりも高いZr(IV)抽出能力を示すことが明らかとなった。

The extraction and separation of Zr(IV) as a major fission product from aqueous HNO$$_{3}$$ solutions have been investigated extensively because the presence of Zr in the TBP-based PUREX process for reprocessing spent nuclear fuel is problematic. Moreover, the formation of liquid-liquid (water, oil) interfacial cruds or a third phase during Zr extraction by TBP from HNO$$_{3}$$ aqueous solution occurs with a high metal loading in the organic phase. In this study, we develop a fluoroalkylated phosphate (TFP) for Zr(IV) extraction to increase the extractability and prevent third-phase formation. We investigated the extraction performance and mechanism of TFP extraction of Zr(IV) from HNO$$_{3}$$ solutions into perfluorohexane and compared them with the conventional organic extraction system using TBP in n-octane. The Zr(IV) extraction strength of TFP in the fluorinated diluent perfluorohexane was much higher than that of TBP in n-octane.

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