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X-ray absorption study of molten uranium chloride system

溶融ウラン塩化物のXAFS研究

岡本 芳浩; 赤堀 光雄; 伊藤 昭憲; 小川 徹

Okamoto, Yoshihiro; Akabori, Mitsuo; Ito, Akinori; Ogawa, Toru

LiCl-KCl共晶塩中の、UCl$$_3$$融体の局所構造について、U原子L$$_3$$吸収端XAFS測定によって調べた。XAFS測定は、高エネルギー加速器研究機構の放射光実験施設BL27Bで実施した。ウラン水素化物の塩化によって調製した、UCl$$_4$$を亜鉛粉末で還元してUCl$$_3$$を得た。カーブフィッティング解析の結果、最近接U$$^{3+}$$-Cl$$^-$$相関に関する構造情報を得た。MD計算とXAFSシミュレーションコードFEFF8の併用から、最近接U$$^{3+}$$-Cl$$^-$$相関の相互作用について評価した。また、いくつかのウランハロゲン化物のXANES測定を行い、そのシフトから原子価について評価した。

We report local structural features of molten UCl$$_3$$ with LiCl-KCl eutectic probed by the U L$$_3$$-edge XAFS(X-ray absorption fine structure). The XAFS measurements were performed in a transmission mode at the BL27B station of the Photon Factory(High Energy Accelerator Organization, Tsukuba, JAPAN). Sample prepared by chlorination of uranium hydride and then reduction with zinc powder was sealed in a quartz cell under reduced pressure. The nearest U$$^{3+}$$-Cl$$^-$$ distance and the coordination number of Cl$$^-$$ around U$$^{3+}$$ ion were obtained by a curve fitting of the 1st shell XAFS function k$$^3$$$$chi$$(k). The pair potential in the U$$^{3+}$$-Cl$$^-$$ correlation was evaluated from XAFS simulation by combinational use of the MD and the FEFF8. In addition, valence state of uranium in the melt was evaluated by XANES(X-ray absorption near edge structure) spectra.

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