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Deposition Behavior of Supersaturated Silicic Acid in the Condition of Relatively High Ca or Na Concentration

机译:在相对高Ca或Na浓度的情况下,过饱和硅酸的沉积行为

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Around the radioactive waste repository, the pH of the groundwater greatly changes from 8 to 13 and the groundwater contains a relatively large quantity of calcium (Ca) and sodium (Na) ions due to cementitious materials used for the construction of the geological disposal system. Under such conditions, the deposition behavior of silicic acid is one of the key factors for the migration assessment of radionucltdes. The deposition and precipitation of silicic acid with the change of pH and coexisting ions may contribute to the clogging in flow paths, which is expected as the retardation effect of radionuclides. Thus, this study focused on the deposition behavior of silicic acid under the condition of relatively high Ca or Na concentration. In the experiments, Na_2SiO_3 solution (250 ml, 14 mM, pH>10, 298 K) was prepared in a polyethylene vessel containing amorphous silica powder (0.5 g) as the solid phase. Then, a buffer solution (to adjust to 8 in pH), HNO_3, and Ca(NO_3)_2 as Ca ions or NaCl as Na ions were sequentially added. Such a silicic acid solution becomes supersaturated, gradually forming colloidal silicic-acid and/or the deposit on the solid surface. In this study, the both concentrations of soluble and colloidal silicic-acid were monitored over a 40-day period. As a result, the deposition rate of silicic acid decreased with up to 5 mM in Ca ions. Besides, Na ions with up to 0.1 M slightly increased the deposition rate. Under the conditions of [Na~+]>0.1 M or [Ca~(2+)]>5 mM, the supersaturated silicic acid immediately deposited. These suggest that Na or Ca ions strongly affect the deposition behavior of supersaturated silicic-acid, depending on the surface alteration of solid phase, the change of zeta potential and the decrease of water-activity due to the addition of electrolytes (coexisting ions).
机译:在放射性废物储存库周围,地下水的pH从8到13且由于用于构造地质处理系统的水泥材料而导致的地下水含有相对大量的钙(Ca)和钠(Na)离子。在这种条件下,硅酸的沉积行为是放射性核心迁移评估的关键因素之一。硅酸与pH的变化和共存离子的沉积和沉积可以有助于流动路径的堵塞,这预期为放射性核素的延迟效果。因此,该研究的重点是在相对高Ca或Na浓度的条件下硅酸的沉积行为。在实验中,在含有非晶二氧化硅粉末(0.5g)的聚乙烯容器中制备Na_2SiO_3溶液(250mL,14mM,pH> 10,298k),为固相。然后,将缓冲液(调整到pH值8),HNO_3,和Ca(NO_3)_2如Ca离子或NaCl作为依次加入Na离子。这种硅酸溶液变得过饱和,逐渐形成胶体硅酸和/或固体表面上的沉积物。在该研究中,在40天的时间内监测可溶性和胶体硅酸的两种浓度。结果,硅酸的沉积速率随高达5mm的Ca离子降低。此外,Na离子高达0.1米略微增加沉积速率。在[Na〜+]> 0.1M或[Ca〜(2 +)]> 5mm的条件下,立即沉积过饱和硅酸。这些表明Na或Ca离子强烈影响超饱和硅酸的沉积行为,这取决于固相的表面改变,Zeta电位的变化和由于添加电解质(共存离子)的水 - 活性降低。

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