Inhibition of U(VI) Reduction by Synthetic and Natural Pyrite

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• 作者：Zhuanwei Yang ; Mingliang Kang ; Bin Ma ; Jinglin Xie ; Fanrong Chen ; Laurent Charlet ; Chunli Liu
• 刊名：Environmental Science & Technology
• 出版年：2014
• 出版时间：September 16, 2014
• 年：2014
• 卷：48
• 期：18
• 页码：10716-10724
• 全文大小：566K
• ISSN：1520-5851

文摘

Reductive precipitation is an effective method of attenuating the mobility of uranium (U) in subsurface environments. The reduction of U(VI) by synthetic and naturally occurring pyrite was investigated at pH 3.0鈥?.5. In contrast to thermodynamic calculations that were used to predict UO₂(s) precipitation, a mixed U(IV) and U(VI) product (e.g., U₃O₈/U₄O₉/U₃O₇) was only observed at pH 6.21鈥?.63 and 4.52鈥?.83 for synthetic and natural pyrite, respectively. Under acidic conditions, the reduction of UO₂²⁺ by surface-associated Fe²⁺ may not be favored because the mineral surface is nearly neutral or not negative enough. At high pH, the sorption of negatively charged U(VI) species is not favored on the negatively charged mineral surface. Thus, the redox reaction is not favored. Trace elements generally contained within the natural pyrite structure can affect the reactivity of pyrite and lead to a different result between the natural and synthetic pyrite. Because UO₂(s) is extremely redox-sensitive toward U(VI), the observed UO_2+x(s) phase reduction product indicates a surface reaction that is largely controlled by reaction kinetics and pyrite surface chemistry. These factors may explain why most laboratory experiments have observed incomplete U(VI) reduction on Fe(II)-bearing minerals.