Mechanistic understanding and prediction of solute adsorption from fluids onto mineral surfaces is relevant for many natural and technical processes. Mineral surfaces in natural systems are often exposed to fluids at non-equilibrium conditions resulting in surface dissolution reactions. Such reactions cause the formation of surface nanotopography and, consequently, the exposure of different types of surface atoms. The quantitative effect of nanotopography on the efficiency of adsorption reactions at crystal surfaces is not known. Using kinetic Monte Carlo simulations, we combined a model of muscovite (001) face dissolution with a consequent model of radionuclide adsorption on the rough mineral surface. The model considers three different adsorption sites based on the muscovite surface cations: silicon, tetrahedral, and octahedral aluminum. Two different nanotopography configurations are investigated, both showing similar adsorption behavior. Octahedral aluminum surface atoms defined by having the highest reactivity toward adsorption are exposed solely on steps and pits on the muscovite (001) face. Thus, their availability directly depends on the surface nanotopography. The model results show the need for a more precise parameterization of surface site-specific adsorption, taking into account the coordination of the involved surface cation such as kink, step, or terrace sites.

中文翻译：

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动力学蒙特卡洛模拟研究白云母（001）表面纳米形貌对放射性核素吸附的影响

机械理解和预测从流体到矿物表面的溶质吸附与许多自然和技术过程有关。天然系统中的矿物表面经常在非平衡条件下暴露于流体中，从而导致表面溶解反应。此类反应导致表面纳米形貌的形成，并因此导致不同类型表面原子的暴露。纳米形貌对晶体表面吸附反应效率的定量影响尚不清楚。使用动力学蒙特卡洛模拟，我们将白云母（001）面溶解模型与放射性核素在粗糙矿物表面上的吸附模型相结合。该模型根据白云母表面阳离子考虑了三个不同的吸附位点：硅，四面体和八面体铝。研究了两种不同的纳米形貌配置，均显示出相似的吸附行为。通过对吸附具有最高反应性而定义的八面体铝表面原子仅暴露在白云母（001）面上的台阶和凹坑上。因此，它们的可用性直接取决于表面纳米形貌。模型结果表明，需要考虑到所涉及的表面阳离子（如扭结，台阶或平台部位）的配位，需要对表面特定位置的吸附进行更精确的参数化。它们的可用性直接取决于表面纳米形貌。模型结果表明，需要考虑到所涉及的表面阳离子（如扭结，台阶或平台部位）的配位，需要对表面特定位置的吸附进行更精确的参数化。它们的可用性直接取决于表面纳米形貌。模型结果表明，需要考虑到所涉及的表面阳离子（如扭结，台阶或平台部位）的配位，需要对表面特定位置的吸附进行更精确的参数化。