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高選択・制御性沈殿剤による高度化沈殿法再処理システムの開発,11; ピロリドン誘導体を有する硝酸プルトニル錯体の構造解析

Development of advanced reprocessing system using high selective and controllable precipitants, 11; Structural analyses of Pu(VI) nitrate complexes with pyrrolidone derivatives

Kim, S.-Y.; 芳賀 芳範   ; 山本 悦嗣  ; 川田 善尚; 森田 泰治  ; 池田 泰久*; 西村 建二*

Kim, S.-Y.; Haga, Yoshinori; Yamamoto, Etsuji; Kawata, Yoshihisa; Morita, Yasuji; Ikeda, Yasuhisa*; Nishimura, Kenji*

ピロリドン誘導体であるN-シクロヘキシル-2-ピロリドン(NCP)、N-ネオペンチル-2-ピロリドン(NNpP)を配位した硝酸プルトニル錯体の赤外吸収スペクトル測定及び単結晶X線構造解析を行い、PuO$$_{2}$$(NO$$_{3}$$)$$_{2}$$(NCP)$$_{2}$$及びPuO$$_{2}$$(NO$$_{3}$$)$$_{2}$$(NNpP)$$_{2}$$の分子及び結晶構造を明らかにした。PuO$$_{2}$$(NO$$_{3}$$)$$_{2}$$(NCP)$$_{2}$$及びPuO$$_{2}$$(NO$$_{3}$$)$$_{2}$$(NNpP)$$_{2}$$の錯体は、Pu(VI)溶液とPuの2倍量のNCPを加え、溶液を撹拌することで沈殿を析出させて調製した。PuO$$_{2}$$(NO$$_{3}$$)$$_{2}$$(NCP)$$_{2}$$及びPuO$$_{2}$$(NO$$_{3}$$)$$_{2}$$(NNpP)$$_{2}$$の単結晶X線構造解析の結果、いずれの錯体においても、NCP又はNNpP及びNO$$_{3}$$ $$^{-}$$をそれぞれ2個ずつエカトリアル面に配位した六方両錐型の結晶構造を持ち、Pu=O$$_{yl}$$;$$underline{1.727-1.731}$$${AA}$, PuO$$_{L}$$;$$underline{2.377-2.390}$$${AA}$, Pu-O$$_{NO3}$$;$$underline{2.490-2.507}$$${AA}$といった結合距離を有することが明らかになった。

The crystal structure of plutonyl(VI) nitrate complexes, PuO$$_{2}$$(NO$$_{3}$$)$$_{2}$$(L)$$_{2}$$ [L=N-cyclohexyl-2-pyrrolidone (NCP), N-Neopentyl-2-pyrrolidone (NNpP)] have been prepared by mixing PuO$$_{2}$$(NO$$_{3}$$)$$_{2}$$ and L in an aqueous nitric acid solution and its crystal structure was determined using X-ray diffractometry and confirmed by IR spectroscopy. The plutonyl(VI) nitrate complexes with L normally have a composition of PuO$$_{2}$$(NO$$_{3}$$)$$_{2}$$(L)$$_{2}$$, which shows common structural features, i.e., the plutonyl ion is surrounded by four oxygen atoms from two NO$$_{3}$$ $$^{-}$$ and two donating atoms of two L in its equatorial plane. X-ray diffraction study reveals that average distances between plutonium atom and plutonyl-, nitrate-, and carbonyl- oxygen atoms are 1.727-1.731 ${AA}$, 2.490-2.507 ${AA}$, 2.377-2.390 ${AA}$, respectively.

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