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• W2795330824 abstract "Simulation of gas adsorption on graphite is commonly carried out using a model that assumes that graphite has an energetically homogeneous surface, constant interlayer spacing, and isotropically polarizable carbon atoms. This simple model fails to describe experimental isotherms and isosteric heats for many gas/graphite pairs. In this paper, we investigate the adsorption of krypton and methane on graphite, using a recently developed molecular model for graphite, that has been shown to improve the description of experimental isotherms and isosteric heats for nitrogen and argon.(1−3) Although the collision diameters of krypton and methane are almost the same, their isotherms and heats are significantly different. With the aid of detailed microscopic analysis, we establish the mechanism underlying the transitions in adsorbate loading as well as the origin of the spike in the experimental isosteric heat versus loading for methane and krypton. The first adsorbate layer of both adsorbates exhibits the transition from a 2D-fluid to a commensurate (C) state; but only krypton shows a subsequent transition to incommensurate (IC) packing before the onset of the second layer. However, the first adsorbate layer of the methane isotherm does also undergo this transition, but only after the second layer has been formed at higher temperatures (T > 87 K). This is explained by the difference between the intermolecular spacing in the C-packed lattice and in the IC-lattice. The difference is smaller for methane than for krypton, making it more difficult for methane to achieve IC-packing and it is also reflected in the isosteric heat versus loading (heat curve). The heat curves for both adsorbates exhibit an increase in the isosteric heat at submonolayer coverage and reach a maximum at the coverage corresponding to C-packing at temperatures far below the triple point. As the temperature is increased, the isosteric heat also increases to a maximum at a loading less than the C-packing, followed by a cusp due to the onset of the second layer, prior to the spike at the C-packing. The difference between the two adsorbates is shown by the appearance of an additional spike for krypton when the C–IC transition occurs. These heat spikes for Kr due to C-packing and IC-packing shift to higher loading and have smaller magnitudes at higher temperatures because of the contributions from higher layers." @default.
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• W2795330824 date "2018-03-27" @default.
• W2795330824 modified "2023-09-26" @default.
• W2795330824 title "Comparison of the Adsorption Transitions of Methane and Krypton on Graphite at Sub-Monolayer Coverage" @default.
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• W2795330824 doi "https://doi.org/10.1021/acs.jpcc.8b00535" @default.
• W2795330824 hasPublicationYear "2018" @default.
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