Evaluation of the Behavior of Uranium Peroxocarbonate Complexes in Na鈥揢(VI)鈥揅O3鈥揙H鈥揌2O2 Solutions by Raman Spectroscopy

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• 作者：Kwang-Wook Kim ; Euo-Chang Jung ; Keun-Young Lee ; Hye-Ryun Cho ; Eil-Hee Lee ; Dong-Yong Chung
• 刊名：The Journal of Physical Chemistry A
• 出版年：2012
• 出版时间：December 13, 2012
• 年：2012
• 卷：116
• 期：49
• 页码：12024-12031
• 全文大小：501K
• 年卷期：v.116,no.49(December 13, 2012)
• ISSN：1520-5215

文摘

In this work, the formation of uranium species and their stabilities in Na鈥揢(VI)鈥揅O₃鈥揙H鈥揌₂O₂ solutions at different pHs are studied by Raman spectroscopy. In this solution, the UO₂(O₂)(CO₃)₂^{4鈥?/sup> species was formed together with three other uranium species of UO₂(O₂)₂2鈥?/sup>, UO₂(CO₃)₃4鈥?/sup>, and a speculated uranium species of the uranyl carbonate hydroxide complex, UO₂(CO₃)_x(OH)_y2鈥?x鈥?i>y, which showed remarkable Raman peaks at approximately 769, 848, 811, and 727 cm鈥?, respectively. The UO₂(O₂)(CO₃)₂4鈥?/sup> species disappeared at pH conditions where bicarbonate dominated, and its Raman peak could be clearly observed in only a narrow pH range from approximately 9 to 12. When the pH of the solution increased further, the UO₂(O₂)(CO₃)₂4鈥?/sup> species changed to UO₂(CO₃)₃4鈥?/sup> and the UO₂(CO₃)_x(OH)_y2鈥?x鈥?i>y species. Moreover, the UO₂(O₂)(CO₃)₂4鈥?/sup> species continuously decomposed into uranyl tricarbonate in the carbonate solution at an elevated temperature because of the instability of the peroxide ion, O₂2鈥?/sup>, in alkaline conditions.}