Interaction between Gaomiaozi bentonite colloid and uranium

Shan Zhu , Zhaomin Tan , Xin Wei , Qiang Tian , Zhichao Zhu , Fang Yang , Mark Julian Henderson , Minhao Yan
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Abstract

In a deep geological repository system, the presence of clay colloids in the geological disposal medium is considered to be a potential factor promoting nuclide migration. In this study, Gaomiaozi bentonite colloid (GMZC) was extracted using the gravity sedimentation method, and its interaction with U(VI) at neutral pH was studied. Small angle X-ray scattering (SAXS), X-ray photoelectron spectroscopy (XPS), dynamic light scattering, and other characterizations methods were used to analyze and observe the microstructure and agglomeration morphology of the bentonite colloidal particles before and after the reaction with U(VI) at the macro-meso-microscopic level. The XPS results indicate that the U(VI) reacted with the Si–O and Al–O on the GMZC particle surfaces at room temperature, and the hydrolyzed product of the U(VI) covered the colloidal surfaces in the neutral water environment, resulting in a decrease in the absolute zeta potential (from ∼31 mV to ∼19 mV). The hydrodynamic diameter of the colloidal particles did not change significantly (∼336 nm–∼360 nm), but the small-angle scattering data revealed that the fractal dimension was larger after the reaction (∼2.8–∼3.1), indicating particle agglomeration. About 14% of the GMZC particles were precipitated after reacting with the U(VI). When the temperature was increased to 55 °C and 85 °C, the precipitation did not change significantly, but the fractal dimension of the mixed system increased (from ∼3.1 to ∼3.6), and the d001 peak was not observed in the SAXS results. When the temperature was decreased by 25 °C, the hydrodynamic diameter of the zeta potential and SAXS image both returned to the level before the temperature increase, indicating that the unstable change in the colloidal system caused by the temperature increase was reversible.

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高庙子膨润土胶体与铀的相互作用
在深部地质处置体系中,地质处置介质中粘土胶体的存在被认为是促进核素迁移的潜在因素。本研究采用重力沉淀法提取高庙子膨润土胶体(GMZC),并研究其在中性pH下与U(VI)的相互作用。采用小角x射线散射(SAXS)、x射线光电子能谱(XPS)、动态光散射等表征方法,在宏细观水平上分析观察了膨润土胶体颗粒与U(VI)反应前后的微观结构和团聚形态。XPS结果表明,在室温下,U(VI)与Si-O和Al-O在GMZC颗粒表面发生反应,U(VI)的水解产物覆盖在中性水环境的胶体表面,导致绝对zeta电位下降(从~ 31 mV降至~ 19 mV)。胶体颗粒的水动力直径变化不明显(~ 336 nm ~ ~ 360 nm),但小角散射数据显示,反应后的分形维数增大(~ 2.8 ~ ~ 3.1),表明颗粒聚集。约14%的GMZC颗粒与U(VI)反应后析出。当温度升高到55℃和85℃时,降水变化不明显,但混合体系的分形维数增加(从~ 3.1增加到~ 3.6),SAXS结果中未观察到d001峰。当温度降低25℃时,zeta电位的流体动力直径和SAXS图像均恢复到温度升高前的水平,表明温度升高引起的胶体体系的不稳定变化是可逆的。
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