Reactive Transport of U and V from Abandoned Uranium Mine Wastes.

Reactive Transport of U and V from Abandoned Uranium Mine Wastes.
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DOI:
10.1021/acs.est.7b03823
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发表时间:
2017-11-07
影响因子:
11.4
通讯作者:
Cerrato JM
Cerrato JM
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
Avasarala S;Lichtner PC;Ali AS;González-Pinzón R;Blake JM;Cerrato JM

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通过将流动柱实验与反应输运模型和电子显微镜相结合,研究了从亚利桑那州Blue Gap/Tachee Claim-28矿区收集的废弃矿山废物中铀(U)和钒(V)的反应输运。在pH 7.9的条件下,矿山废弃物在流通柱中顺序反应(10 mM HCO 3 −)和pH 3.4(10 mM CH 3COOH),以评估在Blue Gap/Tachee遇到的环境相关条件对U和V释放的影响。Blue Gap/Tachee主要铀酰钒酸盐(U-V)矿物溶解的反应速率常数(km)。Tachee是由反应输运软件PFLOTRAN模拟得到的。对于pH 7.9(km = 4.8 × 10−13 mol cm−2 s−1)和pH 3.4(km = 3.2 × 10−13 mol cm−2 s−1),估计的反应速率常数在1个数量级以内。然而,在中性附近(Keq = 10−38.65)与酸性pH(Keq = 10−44.81)下,含铀钒矿物的平衡常数(Keq)的估计值相差超过6个数量级。这些结果与电子显微镜数据相结合表明,U和V的释放受水的pH值和含U-V矿物的晶体结构的影响。这项调查的结果具有重要的影响,风险暴露评估,修复和资源回收的U和V的地方,铀-钒的矿物丰富。
The reactive transport of uranium (U) and vanadium(V) from abandoned mine wastes collected from the Blue Gap/Tachee Claim-28 mine site in Arizona was investigated by integrating flow-through column experiments with reactive transport modeling, and electron microscopy. The mine wastes were sequentially reacted in flow-through columns at pH 7.9 (10 mM HCO3−) and pH 3.4 (10 mM CH3COOH) to evaluate the effect of environmentally relevant conditions encountered at Blue Gap/Tachee on the release of U and V. The reaction rate constants (km) for the dissolution of uranyl–vanadate (U–V) minerals predominant at Blue Gap/Tachee were obtained from simulations with the reactive transport software, PFLOTRAN. The estimated reaction rate constants were within 1 order of magnitude for pH 7.9 (km = 4.8 × 10−13 mol cm−2 s−1) and pH 3.4 (km = 3.2 × 10−13 mol cm−2 s−1). However, the estimated equilibrium constants (Keq) for U–V bearing minerals were more than 6 orders of magnitude different for reaction at circumneutral pH (Keq = 10−38.65) compared to acidic pH (Keq = 10−44.81). These results coupled with electron microscopy data suggest that the release of U and V is affected by water pH and the crystalline structure of U–V bearing minerals. The findings from this investigation have important implications for risk exposure assessment, remediation, and resource recovery of U and V in locations where U–V-bearing minerals are abundant.
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