土壤孔隙介质中钚胶体、Sr2+、氚水的运移速率差异:实验和原理研究

    Differences in Transport Velocities of Plutonium Pseudo-Colloids, Sr2+, and Tritiated Water in Soil Porous Media: Experimental and Theoretical Study

    • 摘要: 放射性污染物在地下水中的运移速率是预测其是否对生态环境构成威胁的重要参量。Pu(Ⅳ)吸附于天然胶体表面生成的复合胶体比孔隙水运移速率快的现象已被广泛报道。然而准确取得胶体和孔隙水间相对运移速率的问题仍未解决,以往的单点法仅是一种大致的估计,很多情况下甚至无法使用。为此,完成了混合示踪源(钚胶体、氚水、Sr2+)在土壤孔隙介质中的运移实验(氚水与孔隙水的运移行为一致)。结果表明:钚胶体、氚水(TW)、Sr2+的运移速率关系为v(Pu)>v(TW)>v(Sr2+)。由负电性钚胶体(分布于孔隙通道中心)、电中性氚水(均匀分布于整个孔隙通道)、Sr2+(分布于孔隙通道壁面区域)与负电性孔隙通道壁面间的静电作用差异和抛物线状孔隙水流,推导出v(Pu)/v(TW)和v(Sr2+)/v(TW)的表达式,通过使用穿透曲线上所有数据取得了准确的相对运移速率:v(Pu)/v(TW) = 1.4,v(Sr2+)/v(TW) = 0.58。

       

      Abstract: The transport velocity of radioactive pollutants in groundwater is an important parameter for predicting whether they pose risks to the surrounding ecological environment at nuclear test sites. It has been widely reported that Pu(Ⅳ) adsorbed on the surface of natural colloids(i.e., formation of plutonium pseudo-colloids) has faster transport velocity than that of the porewater in porous media. However, how to accurately obtain the relative transport velocity between colloids and porewater remains unanswered. The previous single-point method(i.e., using only one data point on each of the two breakthrough curves), lack of the theoretical support, is considered as only a rough estimate. This method cannot even be used in many cases. For example, when there is little difference in the transport velocities between colloidal pollutants and tritiated water, the effluent concentration peaks both appear in the same test tube collecting the effluent(i.e., they have the same effluent volume). Note that the transport behavior of tritiated water(an electroneutrally inert tracer) is consistent with that of the porewater. In a long-pulse transport experiment, the breakthrough curves exhibit prolonged plateaus rather than showing concentration peaks. As there is no concentration peak, it is impossible to compare the transport velocity of the two pollutants. In this study, the mixed tracer sources containing plutonium pseudo-colloids, tritiated water, and Sr2+ were injected into a column packed with porous media(soils) to conduct a transport experiment. The column effluent was collected at regular intervals. The breakthrough curves for plutonium pseudo-colloids, tritiated water, and Sr2+ were obtained after their concentrations(or activity) in the effluent were measured. The results show that the transport velocity relationship between plutonium pseudo-colloids, tritiated water(TW), and Sr2+ is v(Pu)>v(TW)>v(Sr2+). The quantitative relationships between relative transport velocities still need to be accurately determined. The negatively charged plutonium pseudo-colloids were electrostatically repelled to the center of the pore channels. The electroneutral tritiated waters were uniformly distributed within the channels. In contrast, the positive Sr2+ ions were electrostatically attracted near the channel walls. Accordingly, the expressions for the relative transport velocities of v(Pu)/v(TW) and v(Sr2+)/v(TW) were deduced based on the parabolic porewater flow and the differences in the electrostatic interactions between plutonium pseudo-colloids, tritiated water, Sr2+, and the negatively charged pore-channel walls. The accurate relative transport velocities were thus determined by using all data from the breakthrough curves of plutonium pseudo-colloids, tritiated water and Sr2+: v(Pu)/v(TW)=1.4, v(Sr2+)/v(TW)=0.58.

       

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