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Redox equilibria of Pu$$^{4+}$$/Pu$$^{3+}$$ and PuO$$_{2}$$$$^{2+}$$/Pu$$^{4+}$$ couples in molten NaCl-CsCl eutectic as measured by absorption spectrophotometry

Nagai, Takayuki; Uehara, Akihiro*; Fujii, Toshiyuki*; Shirai, Osamu*; Myochin, Munetaka; Yamana, Hajimu*

Redox behavior of uranium and plutonium in molten salts is the essential information for establishing an effective reprocessing process with spent MOX fuel. In an oxide electro-winning reprocessing process, the spent nuclear fuel is dissolved into the molten NaCl-CsCl eutectic, and the dissolved U(VI) and Pu(VI) species are reduced to be dioxides by electrolysis. In the present study, formal redox potentials of the Pu$$^{4+}$$/Pu$$^{3+}$$ and PuO$$_{2}$$$$^{2+}$$/Pu$$^{4+}$$ couples in the molten NaCl-CsCl eutectic at 923 K were determined. The fractions of Pu$$^{3+}$$, Pu$$^{4+}$$, and PuO$$_{2}$$$$^{2+}$$ were determined by UV/Vis/NIR absorption spectrophotometry. PuO$$_{2}$$ was dissolved into the molten NaCl-CsCl eutectic by Cl$$_{2}$$$$_{2}$$ gas purging. Valences of plutonium (Pu$$^{0}$$, Pu$$^{3+}$$, Pu$$^{4+}$$, and PuO$$_{2}$$$$^{2+}$$) were controlled by changing the flow rates of Cl$$_{2}$$, O$$_{2}$$, and Ar gases.

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Category:Chemistry, Inorganic & Nuclear

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