Flury Markus, Czigány Szabolcs, Chen Gang, Harsh James B
Department of Crop and Soil Sciences, Center for Multiphase Environmental Research, Washington State University, Pullman, WA 99164, USA.
J Contam Hydrol. 2004 Jul;71(1-4):111-26. doi: 10.1016/j.jconhyd.2003.09.005.
Large amounts of 137Cs have been accidentally released to the subsurface from the Hanford nuclear site in the state of Washington, USA. The cesium-containing liquids varied in ionic strengths, and often had high electrolyte contents, mainly in the form of NaNO3 and NaOH, reaching concentrations up to several moles per liter. In this study, we investigated the effect of ionic strengths on Cs migration through two types of porous media: silica sand and Hanford sediments. Cesium sorption and transport was studied in 1, 10, 100, and 1000 mM NaCl electrolyte solutions at pH 10. Sorption isotherms were constructed from batch equilibrium experiments and the batch-derived sorption parameters were compared with column breakthrough curves. Column transport experiments were analyzed with a two-site equilibrium-nonequilibrium model. Cesium sorption to the silica sand in batch experiments showed a linear sorption isotherm for all ionic strengths, which matched well with the results from the column experiments at 100 and 1000 mM ionic strength; however, the column experiments at 1 and 10 mM ionic strength indicated a nonlinear sorption behavior of Cs to the silica sand. Transport through silica sand occurred under one-site sorption and equilibrium conditions. Cesium sorption to Hanford sediments in both batch and column experiments was best described with a nonlinear Freundlich isotherm. The column experiments indicated that Cs transport in Hanford sediments occurred under two-site equilibrium and nonequilibrium sorption. The effect of ionic strength on Cs transport was much more pronounced in Hanford sediments than in silica sands. Effective retardation factors of Cs during transport through Hanford sediments were reduced by a factor of 10 when the ionic strength increased from 100 to 1000 mM; for silica sand, the effective retardation was reduced by a factor of 10 when ionic strength increased from 1 to 1000 mM. A two order of magnitude change in ionic strength was needed in the silica sand to observe the same change in Cs retardation as in Hanford sediments.
大量的137Cs已从美国华盛顿州的汉福德核设施意外泄漏到地下。含铯液体的离子强度各不相同,且通常含有高电解质含量,主要以NaNO3和NaOH的形式存在,浓度可达每升几摩尔。在本研究中,我们研究了离子强度对铯在两种多孔介质(硅砂和汉福德沉积物)中迁移的影响。在pH值为10的1、10、100和1000 mM NaCl电解质溶液中研究了铯的吸附和迁移。通过批量平衡实验构建吸附等温线,并将批量得出的吸附参数与柱突破曲线进行比较。用双位点平衡 - 非平衡模型分析柱迁移实验。在批量实验中,铯在所有离子强度下对硅砂的吸附均呈现线性吸附等温线,这与100和1000 mM离子强度下的柱实验结果吻合良好;然而,1和10 mM离子强度下的柱实验表明铯对硅砂呈现非线性吸附行为。铯在硅砂中的迁移是在单位点吸附和平衡条件下发生的。在批量和柱实验中,铯对汉福德沉积物的吸附最好用非线性弗伦德利希等温线来描述。柱实验表明,铯在汉福德沉积物中的迁移是在双位点平衡和非平衡吸附条件下发生的。离子强度对铯迁移的影响在汉福德沉积物中比在硅砂中更为显著。当离子强度从100 mM增加到1000 mM时,铯在通过汉福德沉积物迁移过程中的有效阻滞因子降低了10倍;对于硅砂,当离子强度从1 mM增加到1000 mM时,有效阻滞降低了10倍。在硅砂中需要离子强度有两个数量级的变化才能观察到与汉福德沉积物中铯阻滞相同的变化。