A Universal Descriptor for the Entropy of Adsorbed Molecules in Confined Spaces,ACS Central Science

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A Universal Descriptor for the Entropy of Adsorbed Molecules in Confined Spaces
ACS Central Science ( IF 12.7 ) Pub Date : 2018-09-07 00:00:00 , DOI: 10.1021/acscentsci.8b00419
Paul J. Dauenhauer _{1,

2} , Omar A. Abdelrahman _{2,

3}

Affiliation

Confinement of hydrocarbons in nanoscale pockets and pores provides tunable capability for controlling molecules in catalysts, sorbents, and membranes for reaction and separation applications. While computation of the enthalpic interactions of hydrocarbons in confined spaces has improved, understanding and predicting the entropy of confined molecules remains a challenge. Here we show, using a set of nine aluminosilicate zeolite frameworks with broad variation in pore and cavity structure, that the entropy of adsorption can be predicted as a linear combination of rotational and translational entropy. The extent of entropy lost upon adsorption is predicted using only a single material descriptor, the occupiable volume (V_occ). Predictive capability of confined molecular entropy permits an understanding of the relation with adsorption enthalpy, the ability to computationally screen microporous materials, and an understanding of the role of confinement on the kinetics of molecules in confined spaces.

中文翻译：

密闭空间中吸附分子的熵的通用描述子

将碳氢化合物限制在纳米级囊袋和孔隙中可提供可调节的能力，以控制用于反应和分离应用的催化剂，吸附剂和膜中的分子。虽然改进了密闭空间中碳氢化合物的焓相互作用的计算，但了解和预测密闭分子的熵仍然是一个挑战。在这里，我们显示，使用一组九种在孔隙和腔结构中具有广泛变化的铝硅酸盐沸石骨架，可以将吸附熵预测为旋转和平移熵的线性组合。吸附时熵损失的程度仅使用单一的材料描述变量即可占据的体积（V _occ）。有限的分子熵的预测能力使我们能够理解与吸附焓的关系，能够计算筛选微孔材料，并且能够了解有限对有限空间中分子动力学的作用。

更新日期：2018-09-07

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