柠檬酸对Re(VII)在不同压实密度钠基和钙基膨润土中扩散的影响
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O69

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国家自然科学基金项目(面上项目,重点项目,重大项目)


Effect of Citric Acid on Diffusion of Re(VII) in Na+- and Ca2+-bentonite with Different Compacted Density
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The National Natural Science Foundation of China (General Program, Key Program, Major Research Plan)

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    摘要:

    柠檬酸是自然界广泛存在的一种有机酸,可通过络合作用影响放射性核素的迁移。通过贯穿扩散法,研究了柠檬酸对Re(VII)在压实密度为(1.40~1.80)g/cm3的钠基和钙基膨润土中的扩散行为,得到了有效扩散系数(De)和岩石容量因子(α)等扩散系数。结果表明:Re(VII)在钠基和钙基膨润土中扩散的De和α等均随着压实膨润土密度(ρ)的增大而减小;与钙基膨润土相比较,Re(VII)在钠基膨润土中得到的扩散系数较小、吸附分配比较大,表明钠基膨润土的阻滞性能更好;同时加入柠檬酸后Re(VII)在钠基和钙基膨润土中的扩散系数和吸附分配比(Kd)均增大。实验得到膨润土的零点电位点均小于7.0,表明膨润土呈电负性,不易吸附阴离子形式存在的Re(VII)。吸附试验表明加入柠檬酸后,钠基和钙基膨润土对Re(VII)的Kd增大,并随着柠檬酸的浓度增加而增大。通过公式拟合得到Re(VII)在膨润土中扩散的De与有效孔隙率(εacc)均符合Archie定律,其胶结因子(n)分别为2.14和2.19。同时得到扩散的表观扩散系数(Da)与膨润土压实密度均呈指数关系,均符合核素在粘土中扩散的规律。

    Abstract:

    Citric acid is a kind of organic acid widely existing in nature, which can affect the migration of radionuclides through complexation. The diffusion behavior of citric acid to Re(VII) in Na+- and Ca2+- bentonite with compacted densities of (1.40~1.80) g/cm3 was studied by through-diffusion method,the effective diffusion coefficient (De) and rock capacity factor (α) were obtained. The results showed that the De and α of Re(VII) diffused in Na+- and Ca2+- bentonite decreased with increasing density of compacted bentonite. Compared with Ca2+-bentonite, Re(VII) obtained from Na+-bentonite has a smaller diffusion coefficient and a larger adsorption distribution, indicating that Na+-bentonite has a better retarding performance. And the diffusion coefficient and adsorption distribution ratio(Kd) of Re(VII) in Na+-and Ca2+-bentonite increased after adding citric acid. The experimental results showed that the zero potential points of bentonites were all less than 7.0, indicating that the bentonite was electronegative and not easy to absorb Re(VII) in anion form. Adsorption experiments showed that the Kd of Na+-and Ca2+-bentonite to Re(VII) increased after adding citric acid, and as the concentration of citric acid increased. Through formula fitting, the De value and effective porosity (εacc) of Re (VII) diffused in bentonites fitted Archie's law very well, from which the cementation factors(n) obtained are 2.14 and 2.19, respectively. And their apparent diffusion coefficients (Da) are exponentially related to the compacted density of bentonite (ρ). All of them accord the rule of nuclide diffusion in clay.

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张慧,吴昊,罗明标,等. 柠檬酸对Re(VII)在不同压实密度钠基和钙基膨润土中扩散的影响[J]. 科学技术与工程, 2020, 20(21): 8474-8479.
ZHANG Hui, WU Hao, WANG Zhifeng, et al. Effect of Citric Acid on Diffusion of Re(VII) in Na+- and Ca2+-bentonite with Different Compacted Density[J]. Science Technology and Engineering,2020,20(21):8474-8479.

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  • 收稿日期:2019-10-08
  • 最后修改日期:2020-05-28
  • 录用日期:2019-12-24
  • 在线发布日期: 2020-08-18
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