OFM Research-Southwest, Santa Fe, New Mexico 87507, United States.
Environ Sci Technol. 2017 Nov 7;51(21):12385-12393. doi: 10.1021/acs.est.7b03823. Epub 2017 Oct 24.
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 HCO) and pH 3.4 (10 mM CHCOOH) to evaluate the effect of environmentally relevant conditions encountered at Blue Gap/Tachee on the release of U and V. The reaction rate constants (k) 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 (k = 4.8 × 10 mol cm s) and pH 3.4 (k = 3.2 × 10 mol cm s). However, the estimated equilibrium constants (K) for U-V bearing minerals were more than 6 orders of magnitude different for reaction at circumneutral pH (K = 10) compared to acidic pH (K = 10). 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.
从亚利桑那州蓝隙/塔奇矿区 28 号矿废弃矿场采集的废弃矿样中,铀(U)和钒(V)的反应性迁移通过结合流动柱实验、反应性迁移模型和电子显微镜进行了研究。这些废弃矿样在流动柱中先后在 pH7.9(10 mM HCO₃)和 pH3.4(10 mM CH₃COOH)条件下进行反应,以评估蓝隙/塔奇矿区遇到的环境相关条件对 U 和 V 释放的影响。用反应性迁移软件 PFLOTRAN 模拟得到了在蓝隙/塔奇矿区占优势的铀钒(U-V)矿物溶解的反应速率常数(k)。在 pH7.9(k=4.8×10⁻⁵ mol·cm⁻³·s)和 pH3.4(k=3.2×10⁻⁵ mol·cm⁻³·s)条件下,估计的反应速率常数相差一个数量级。然而,对于在中性 pH 条件下(K=10)和酸性 pH 条件下(K=10)反应的 U-V 矿物,其平衡常数(K)相差 6 个数量级以上。这些结果与电子显微镜数据表明,U 和 V 的释放受水 pH 值和 U-V 矿物的结晶结构的影响。这项研究的结果对风险暴露评估、修复以及在 U-V 矿物丰富的地方进行 U 和 V 的资源回收具有重要意义。