Molecular Simulation of the Adsorption of Methane in Engelhard Titanosilicate Frameworks
authors Pillai, RS; Gomes, JRB; Jorge, M
nationality International
journal LANGMUIR
keywords BINARY-MIXTURES; GAS-ADSORPTION; ETS-10; DIFFUSION; SPECTROSCOPY; TEMPERATURE; DIFFRACTION; SILICALITE; SEPARATION; NITROGEN
abstract Molecular simulations were carried out to elucidate the influence of structural heterogeneity and of the presence of extra-framework cations and water molecules on the adsorption of methane in Engelhard titanosilicates, ETS-10 and ETS-4. The simulations employed three different modeling approaches, (i) with fixed cations and water at their single crystal positions, (ii) with fixed cations and water at their optimized positions, and (iii) with mobile extra-framework cations and water molecules. Simulations employing the final two approaches provided a more realistic description of adsorption in these materials, and showed that at least some cations and water molecules are displaced from the crystallographic positions obtained from single crystal data. Upon methane adsorption in the case of ETS-10, the cations move to the large rings, while in the case of ETS-4, the water molecules and cations migrate to more available space in the larger 12-membered ring channels for better accommodation of the methane molecules. For ETS-4, we also considered adsorption in all possible pure polymorph structures and then combined these to provide an estimate of adsorption in a real ETS-4 sample. By comparing simulated adsorption isotherms to experimental data, we were able to show that both the mobility of extra-framework species and the structural heterogeneity should be taken into account for realistic predictions of adsorption in titanosilicate materials.
publisher AMER CHEMICAL SOC
issn 0743-7463
year published 2014
volume 30
issue 25
beginning page 7435
ending page 7446
digital object identifier (doi) 10.1021/la501554v
web of science category Chemistry, Multidisciplinary; Chemistry, Physical; Materials Science, Multidisciplinary
subject category Chemistry; Materials Science
unique article identifier WOS:000338488600022
link 24901733
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