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Prediction of low occupancy sorption of alkanes in silicalite

Journal Article · · Journal of Physical Chemistry; (USA)
DOI:https://doi.org/10.1021/j100367a056· OSTI ID:6712860

Alkane sorption in a pentasil zeolite has been studied through molecular simulations. A series of alkanes, including methane, n-butane, and three hexane isomers, were studied in silicalite by using a detailed atomistic representation that allows for torsion around skeletal bonds. Statistical mechanical principles have been employed to predict sorption equilibria at low occupancy. Henry's constants and isosteric heats of sorption were calculated through the evaluation of configurational integrals with a Monte Carlo integration scheme. Results are in good agreement with experiment. The spatial distribution of sorbate molecules within the pore network, as well as perturbations to their conformation due to confinement in the pores, were determined via Metropolis Monte Carlo algorithm. Simulations of sorbate spatial distributions show that linear alkanes, such as n-butane and n-hexane, prefer to reside in the channels and avoid the channel intersections; on the contrary, bulky side groups in branched alkanes, such as 2- and 3-methylpentane, force these molecules toward the more spacious channel intersections.

OSTI ID:
6712860
Journal Information:
Journal of Physical Chemistry; (USA), Journal Name: Journal of Physical Chemistry; (USA) Vol. 94:4; ISSN 0022-3654; ISSN JPCHA
Country of Publication:
United States
Language:
English