Abstract
The coordination circumstances and redox reactions of UO2 2+ in the aqueous solution concentrated by calcium chloride, such as CaCl2·6H2O (6.9 M CaCl2), were studied by Raman spectroscopy and electrochemical methods. The frequency of the O=U=O symmetrical stretching vibration suggested that the complex formation of UO2 2+ with Cl− leads to the weakening of U=O bond. In the electrochemical measurements, two-step cathodic currents were observed at −0.090 and −0.4 V (vs. Ag|AgCl) corresponding to the reduction of UO2 2+ to UO2 + and that of UO2 + to UO2, respectively. It was found that UO2 + formed at first cathodic current was disproportionated to form UO2 2+ and UO2. The UO2 was identified by X-ray diffraction analysis. Electrolytic deposition of UO2 was observed in 6.9–4.7 M CaCl2 and in 14 M LiCl. When small amount of proton, i.e., 0.005 M was coexisted in 6.9 M CaCl2, UO2 2+ was reduced to form U4+ instead of UO2.
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