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Density Functional Theory Formulation for Fluid Adsorption on Correlated Random Surfaces

机译:相关系统上流体吸附的密度泛函理论公式   随机曲面

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摘要

We provide novel random surface density functional theory (RSDFT) formulationin the case of geometric heterogeneous surface of solid media which isessential for description of thermodynamic properties of confined fluids. Themajor difference of our theoretical approach from existing ones is stochasticmodel of solid surface which takes into account the correlation properties ofgeometry. The main building blocks are effective fluid-solid potentialdeveloped in work (J. Stat. Phys, 2017,167(6), 1519-1545) and geometry basedmodification of Helmholtz free energy for Lennard-Jones fluids. Efficiency ofRSDFT is demonstrated in calculation of argon and nitrogen low temperatureadsorption on real heterogeneous surfaces (BP280 carbon black). These resultsare in good agreement with experimental data published in the literature. Alsoseveral models of corrugated materials are developed in the framework of RSDFT.Numerical analysis demonstrates strong influence of surface roughnesscharacteristics on adsorption isotherms. Thus developed formalism providesconnection between rigorous description of stochastic surface and confinedfluids thermodynamics.
机译:在固体介质的几何异质表面的情况下,我们提供了新颖的随机表面密度泛函理论(RSDFT)公式化,这对于描述承压流体的热力学性质是必不可少的。我们的理论方法与现有方法的主要区别在于考虑了几何相关性的固体表面随机模型。主要组成部分是在工作中开发的有效流体-固体潜能(J.Stat.Phys,2017,167(6),1519-1545)和Lennard-Jones流体基于亥姆霍兹自由能的几何学修饰。 RSDFT的效率在实际异质表面(BP280炭黑)上氩和氮低温吸附的计算中得到了证明。这些结果与文献中发表的实验数据非常吻合。在RSDFT框架内还开发了几种瓦楞纸模型。数值分析表明,表面粗糙度特性对吸附等温线有很大影响。这样发展起来的形式主义提供了对随机表面的严格描述与有限流体热力学之间的联系。

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