Prediction of permeation properties of CO2 and N2 through silicalite via molecular simulations

Makrodimitris, K; Papadopoulos, GK; Theodorou, DN

dc.contributor.author	Makrodimitris, K	en
dc.contributor.author	Papadopoulos, GK	en
dc.contributor.author	Theodorou, DN	en
dc.date.accessioned	2014-03-01T01:16:58Z
dc.date.available	2014-03-01T01:16:58Z
dc.date.issued	2001	en
dc.identifier.issn	1089-5647	en
dc.identifier.uri	https://dspace.lib.ntua.gr/xmlui/handle/123456789/14294
dc.subject	Molecular Simulation	en
dc.subject.classification	Chemistry, Physical	en
dc.subject.other	Carbon dioxide	en
dc.subject.other	Computer simulation	en
dc.subject.other	Isotherms	en
dc.subject.other	Monte Carlo methods	en
dc.subject.other	Nitrogen	en
dc.subject.other	Sorption	en
dc.subject.other	Permeation properties	en
dc.subject.other	Molecular dynamics	en
dc.title	Prediction of permeation properties of CO2 and N2 through silicalite via molecular simulations	en
heal.type	journalArticle	en
heal.identifier.primary	10.1021/jp002866x	en
heal.identifier.secondary	http://dx.doi.org/10.1021/jp002866x	en
heal.language	English	en
heal.publicationDate	2001	en
heal.abstract	The sorption isotherms and self-diffusivities of CO2 and N-2 in silicalite have been calculated via grand canonical Monte Carlo and equilibrium molecular dynamics simulations over a wide range of occupancies, using various force fields proposed in the literature. Predictions for the sorption thermodynamics are in very favorable agreement with the experiment, especially when detailed point-charge models are used to represent the interaction of the quadrupole moments of the sorbate molecules with the lattice field and with each other. They indicate that the zeolite cannot be in its para (P2(1)2(1)2(1)) form under the conditions of the measurements. Permeabilities corresponding to a perfectly crystalline membrane have been estimated for CO2 and N-2, as well as for methane, examined in past simulation work, from the predicted sorption isotherms and low-occupancy self-diffusivities by invoking the Darken equation. The ratios of pure component permeabilities obtained in this way agree very well with actual macroscopic values obtained from carrying out permeation measurements for the different pure sorbates in the same silicalite membrane. Absolute magnitudes of the permeabilities, however, exceed by more than 2 orders of magnitude the reported macroscopic values, which themselves vary widely among different experimental investigations. The large, morphology-dependent nonuniformity in membrane thickness of actual supported silicalite membranes is proposed as a plausible reason for this disparity.	en
heal.publisher	AMER CHEMICAL SOC	en
heal.journalName	Journal of Physical Chemistry B	en
dc.identifier.doi	10.1021/jp002866x	en
dc.identifier.isi	ISI:000166695900007	en
dc.identifier.volume	105	en
dc.identifier.issue	4	en
dc.identifier.spage	777	en
dc.identifier.epage	788	en