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扩展RSA模型在部分覆盖表面颗粒沉积研究中的应用。

Application of the extended RSA models in studies of particle deposition at partially covered surfaces.

作者信息

Weroński Paweł

机构信息

Theoretical Division and Center for Nonlinear Studies, Los Alamos National Laboratory, Los Alamos, NM 87545, USA.

出版信息

Adv Colloid Interface Sci. 2005 Dec 30;118(1-3):1-24. doi: 10.1016/j.cis.2005.03.002. Epub 2005 Aug 8.

Abstract

This paper reviews the application of the extended random sequential adsorption (RSA) approaches to the modeling of colloid-particle deposition (irreversible adsorption) on surfaces precovered with smaller particles. Hard (noninteracting) particle systems are discussed first. We report on the numerical simulations we performed to determine the available surface function, jamming coverage, and pair-correlation function of the larger particles. We demonstrate the effect of the particle size ratio and the small particle surface coverage. We found that the numerical results were in reasonable agreement with the formula stemming from the scaled-particle theory in 2D with a modification for the sphere geometry. Next, we discuss three approximate models of adsorption allowing electrostatic interaction of colloid particles at a charged interface, employing a many-body superposition approximation. We describe two approaches of the effective hard-particle approximation next. We demonstrate the application of the effective hard-particle concept to the bimodal systems and present the effect of electrolyte concentration on the effective particle size ratio. We present the numerical results obtained from the theoretical models of soft-particle adsorption at precovered surfaces. We used the effective hard-particle approximation to determine the corresponding simpler systems of particles, namely the system of hard spheres and the system of hard discs at equilibrium. We performed numerical computations to determine the effective minimum particle surface-to-surface distance, available surface function, jamming coverage, and pair-correlation function of the larger particles at various electrolyte ionic strengths and particle size ratios. The numerical results obtained in the low-surface coverage limit were in good agreement with the formula stemming from the scaled-particle theory with a modification for the sphere geometry and electrostatic interaction. We compared the results of numerical computations of the effective minimum particle surface-to-surface distance obtained using the 2D, 3D, and curvilinear trajectory model. The results obtained with the 3D and curvilinear trajectory models indicate that large-particle/substrate attractive interaction significantly reduces the kinetic barrier to large, charged-particle adsorption at a surface precovered with small, like-charged particles. The available surface function and jamming-coverage values predicted using the simplified 3D and the more sophisticated curvilinear trajectory models are similar, while the results obtained with the 2D model differ significantly. The pair-correlation function suggests different structures of monolayers obtained with the three models. Unlike the three models of the electrostatic interaction, both effective hard-particle approximations give almost identical results. Results of this research clearly suggest that the extended RSA approaches can fruitfully be exploited for numerical simulations of colloid-particle adsorption at precovered surfaces, allowing the investigation of both hard and soft-particle systems.

摘要

本文综述了扩展随机顺序吸附(RSA)方法在模拟胶体颗粒在预先覆盖有较小颗粒的表面上的沉积(不可逆吸附)方面的应用。首先讨论了硬(非相互作用)颗粒系统。我们报告了为确定较大颗粒的可用表面函数、堵塞覆盖率和对关联函数而进行的数值模拟。我们展示了颗粒尺寸比和小颗粒表面覆盖率的影响。我们发现数值结果与二维标度颗粒理论推导的公式合理相符,并对球形几何形状进行了修正。接下来,我们讨论了三种允许胶体颗粒在带电界面处发生静电相互作用的吸附近似模型,采用了多体叠加近似。我们接下来描述了有效硬颗粒近似的两种方法。我们展示了有效硬颗粒概念在双峰系统中的应用,并给出了电解质浓度对有效颗粒尺寸比的影响。我们展示了从预先覆盖表面上软颗粒吸附的理论模型获得的数值结果。我们使用有效硬颗粒近似来确定相应的更简单的颗粒系统,即平衡状态下的硬球系统和硬盘系统。我们进行了数值计算,以确定在各种电解质离子强度和颗粒尺寸比下较大颗粒的有效最小颗粒表面到表面距离、可用表面函数、堵塞覆盖率和对关联函数。在低表面覆盖率极限下获得的数值结果与经过球形几何形状和静电相互作用修正的标度颗粒理论推导的公式高度吻合。我们比较了使用二维、三维和曲线轨迹模型获得的有效最小颗粒表面到表面距离的数值计算结果。三维和曲线轨迹模型获得的结果表明,大颗粒/基质的吸引相互作用显著降低了大带电颗粒在预先覆盖有小的同电荷颗粒的表面上吸附的动力学势垒。使用简化的三维模型和更复杂的曲线轨迹模型预测的可用表面函数和堵塞覆盖率值相似,而二维模型获得的结果有显著差异。对关联函数表明三种模型获得的单层结构不同。与三种静电相互作用模型不同,两种有效硬颗粒近似给出的结果几乎相同。这项研究的结果清楚地表明,扩展的RSA方法可有效地用于数值模拟预先覆盖表面上的胶体颗粒吸附,从而能够研究硬颗粒和软颗粒系统。

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