APPLICATION OF SURFACE COMPLEXATION AND ION EXCHANGE MODELLING FOR THE ESTIMATION OF BENTONITE SORPTION CAPACITY ON SELECTED RADIONUCLIDES UNDER POSSIBLE GEOLOGICAL DISPOSAL CONDITIONS IN LITHUANIA

V. Vaitkevičienė, A. Narkuniene
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Abstract

Designing a repository for radioactive waste as a multi-barrier system with predefined multiple safety functions provides for the protection of people and environment from the harmful effect of the ionising radiation of radionuclides once released from high-level radioactive waste. The multi-barrier system is comprised of the engineered barrier system (EBS) and its surrounding natural environment. Because of the high retention capacity for the radionuclides, various forms of bentonite are usually considered as a part of the EBS in the design of radioactive waste repositories. Laboratory batch experiments with natural sediments illustrate that the sorption (and K d values) is sensitive to aqueous chemical conditions, including the pH and the dissolved carbonate concentration as well as the mineralogy and surface area of the bentonite buffer. The cations considered for the study were chosen as covering a representative range of cations behaviour: from a weakly sorbed cation Cs(I) to moderately sorbed cation the Ni(II) and strongly sorbed cation, Eu(III). In this study, a potential retardation of sorbing radionuclides (Cs, Ni, Eu) as a function of aqueous chemical conditions in the groundwater of the Lithuanian crystalline basement contacting the bentonite material was estimated for the first time. The ion exchange and surface complexation models (SPNE/CE) and the computer program PHREEQC (USA) were applied for modelling the interaction within the radionuclide/water/bentonite system. The modelling of the K d values under different pH conditions and a given partial pressure of carbon dioxide in the gas phase were performed. The highest value of K d in the pCO 2 open system and the strongest sorption dependence on pCO 2 was estimated for Eu(I) among radionuclides being studied. There was estimated only a slight change in K d values with respect to the temperature. DOI: http://dx.doi.org/10.5755/j01.ct.68.1.18875
应用表面络合和离子交换模型估计在立陶宛可能的地质处置条件下膨润土对选定放射性核素的吸附能力
将放射性废物储存库设计为具有预先确定的多种安全功能的多屏障系统,可保护人类和环境免受高放射性废物释放的放射性核素电离辐射的有害影响。多屏障系统由工程屏障系统(EBS)及其周围的自然环境组成。由于各种形式的膨润土对放射性核素具有较高的保留能力,因此在放射性废物储存库的设计中,通常将其作为EBS的一部分。自然沉积物的实验室批量实验表明,吸附(和K - d值)对水化学条件很敏感,包括pH值和溶解的碳酸盐浓度,以及膨润土缓冲液的矿物学和表面积。研究中考虑的阳离子被选择为涵盖了阳离子行为的代表性范围:从弱吸附阳离子Cs(I)到中等吸附阳离子Ni(II)和强吸附阳离子Eu(III)。在这项研究中,首次估计了立陶宛结晶基底地下水中与膨润土材料接触的放射性核素(Cs, Ni, Eu)的潜在吸收延迟作为水化学条件的函数。应用离子交换和表面络合模型(SPNE/CE)和计算机程序PHREEQC (USA)对放射性核素/水/膨润土体系内的相互作用进行了模拟。在不同的pH条件和给定的气相二氧化碳分压下,进行了K - d值的建模。在所研究的放射性核素中,估计Eu(I)在pco2开放体系中的K d值最高,对pco2的吸附依赖性最强。据估计,相对于温度,kd值只有轻微的变化。DOI: http://dx.doi.org/10.5755/j01.ct.68.1.18875
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