On the impact of sorbent mobility on the sorbed phase equilibria and dynamics: A study of methane and carbon dioxide within the zeolite imidazolate framework-8

Pantatosaki, E; Megariotis, G; Pusch, A-K; Chmelik, C; Stallmach, F; Papadopoulos, GK

dc.contributor.author	Pantatosaki, E	en
dc.contributor.author	Megariotis, G	en
dc.contributor.author	Pusch, A-K	en
dc.contributor.author	Chmelik, C	en
dc.contributor.author	Stallmach, F	en
dc.contributor.author	Papadopoulos, GK	en
dc.date.accessioned	2014-03-01T02:11:49Z
dc.date.available	2014-03-01T02:11:49Z
dc.date.issued	2012	en
dc.identifier.issn	19327447	en
dc.identifier.uri	https://dspace.lib.ntua.gr/xmlui/handle/123456789/29952
dc.subject.other	Computer experiment	en
dc.subject.other	Current modeling	en
dc.subject.other	Diffusivities	en
dc.subject.other	Host-guest system	en
dc.subject.other	Imidazolate	en
dc.subject.other	Infrared microscopy	en
dc.subject.other	Isobaric-isothermal	en
dc.subject.other	Kinetic properties	en
dc.subject.other	Maxwell-Stefan	en
dc.subject.other	Modeling results	en
dc.subject.other	Molecular dimensions	en
dc.subject.other	PFG-NMR	en
dc.subject.other	Probability density distribution	en
dc.subject.other	Pulsed-field gradients	en
dc.subject.other	Self-diffusivity	en
dc.subject.other	Simulation prediction	en
dc.subject.other	Sorbate molecules	en
dc.subject.other	Sorbates	en
dc.subject.other	Statistical ensembles	en
dc.subject.other	Transport diffusivity	en
dc.subject.other	Carbon dioxide	en
dc.subject.other	Diffusion	en
dc.subject.other	Dynamics	en
dc.subject.other	Experiments	en
dc.subject.other	Isotherms	en
dc.subject.other	Methane	en
dc.subject.other	Molecular dynamics	en
dc.subject.other	Nuclear magnetic resonance	en
dc.subject.other	Probability density function	en
dc.subject.other	Probability distributions	en
dc.subject.other	Sorption	en
dc.subject.other	Phase equilibria	en
dc.title	On the impact of sorbent mobility on the sorbed phase equilibria and dynamics: A study of methane and carbon dioxide within the zeolite imidazolate framework-8	en
heal.type	journalArticle	en
heal.identifier.primary	10.1021/jp207771s	en
heal.identifier.secondary	http://dx.doi.org/10.1021/jp207771s	en
heal.publicationDate	2012	en
heal.abstract	The presented work aims at exploring the influence of the mobility of the sorbent framework on both the equilibrium and the kinetic properties of the sorbed phase by means of molecular dynamics computer experiments under isochoric-isothermal and isobaric-isothermal statistical ensembles for several host model options, combined by Widom averaging along the entire trajectory of the host-guest system toward rigorously obtained sorbate isotherms within a fully flexible lattice. The methodology is adapted to the study of the self-diffusivity and the collective (Maxwell-Stefan and transport) diffusivities of carbon dioxide (CO2) and methane (CH4) within the zeolite imidazolate framework-8 (ZIF-8). The simulation predictions are compared with measurements from pulsed-field gradient nuclear magnetic resonance (PFG NMR), as well as with recently conducted infrared microscopy (IRM) experiments elaborated on the basis of the current modeling in the flexible ZIF-8. The modeling results reveal a significant influence on sorbate transport exerted by the 2-methilimidazolate ligands surrounding the cage-to-cage entrances, whose apertures are commensurate with the guest molecular dimensions. Moreover, calculations of the singlet probability density distribution of the sorbate molecules at selected regions within the imidazolate framework provide a plausible explanation of the transport diffusivity as a function of sorbate occupancy, measured via IRM. © 2011 American Chemical Society.	en
heal.journalName	Journal of Physical Chemistry C	en
dc.identifier.doi	10.1021/jp207771s	en
dc.identifier.volume	116	en
dc.identifier.issue	1	en
dc.identifier.spage	201	en
dc.identifier.epage	207	en