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添加碱基模拟酸性污染地下水中的铀运移。

Modeling uranium transport in acidic contaminated groundwater with base addition.

机构信息

Key Laboratory of Tibetan Environment Changes and Land Surface Processes, Institute of Tibetan Plateau Research, Chinese Academy of Sciences, P.O. Box 2871, Beijing, 100085, China.

出版信息

J Hazard Mater. 2011 Jun 15;190(1-3):863-8. doi: 10.1016/j.jhazmat.2011.04.022. Epub 2011 Apr 8.

Abstract

This study investigates reactive transport modeling in a column of uranium(VI)-contaminated sediments with base additions in the circulating influent. The groundwater and sediment exhibit oxic conditions with low pH, high concentrations of NO(3)(-), SO(4)(2-), U and various metal cations. Preliminary batch experiments indicate that additions of strong base induce rapid immobilization of U for this material. In the column experiment that is the focus of the present study, effluent groundwater was titrated with NaOH solution in an inflow reservoir before reinjection to gradually increase the solution pH in the column. An equilibrium hydrolysis, precipitation and ion exchange reaction model developed through simulation of the preliminary batch titration experiments predicted faster reduction of aqueous Al than observed in the column experiment. The model was therefore modified to consider reaction kinetics for the precipitation and dissolution processes which are the major mechanism for Al immobilization. The combined kinetic and equilibrium reaction model adequately described variations in pH, aqueous concentrations of metal cations (Al, Ca, Mg, Sr, Mn, Ni, Co), sulfate and U(VI). The experimental and modeling results indicate that U(VI) can be effectively sequestered with controlled base addition due to sorption by slowly precipitated Al with pH-dependent surface charge. The model may prove useful to predict field-scale U(VI) sequestration and remediation effectiveness.

摘要

本研究考察了在添加碱基的循环进水条件下,铀(VI)污染沉积物柱中的反应传输建模。地下水和沉积物呈氧化状态,具有低 pH 值、高浓度的硝酸盐、硫酸盐、U 和各种金属阳离子。初步的批处理实验表明,强碱的添加会导致该材料中 U 的快速固定。在本研究的重点柱实验中,在将地下水重新注入之前,在进水储液器中用 NaOH 溶液滴定,以逐渐增加柱中的溶液 pH 值。通过对初步批处理滴定实验的模拟开发的平衡水解、沉淀和离子交换反应模型预测,水中 Al 的还原速度比在柱实验中观察到的要快。因此,对模型进行了修改,以考虑沉淀和溶解过程的反应动力学,这是 Al 固定的主要机制。综合的动力学和平衡反应模型充分描述了 pH 值、金属阳离子(Al、Ca、Mg、Sr、Mn、Ni、Co)、硫酸盐和 U(VI)在水中的浓度的变化。实验和建模结果表明,由于 pH 值依赖性表面电荷的缓慢沉淀 Al 的吸附,可以通过控制碱基添加有效地将 U(VI)固定。该模型可能有助于预测现场规模的 U(VI)固定和修复效果。

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