title: Ab initio molecular dynamics determination of competitive O₂ vs. N₂ adsorption at open metal sites of M₂(dobdc).
abstract: The separation of oxygen from nitrogen using metal-organic frameworks (MOFs) is of great interest for potential pressure-swing adsorption processes for the generation of purified O2 on industrial scales. This study uses ab initio molecular dynamics (AIMD) simulations to examine for the first time the pure-gas and competitive gas adsorption of O2 and N2 in the M2(dobdc) (M = Cr, Mn, Fe) MOF series with coordinatively unsaturated metal centers. Effects of metal, temperature, and gas composition are explored. This unique application of AIMD allows us to study in detail the adsorption/desorption processes and to visualize the process of multiple guests competitively binding to coordinatively unsaturated metal sites of a MOF.
authors.affiliation: Geochemistry Department, Sandia National Laboratories, Albuquerque, New Mexico 87185-0754, USA.
authors.forename: Marie V
authors.initials: MV
authors.lastname: Parkes
authors.affiliation: Geochemistry Department, Sandia National Laboratories, Albuquerque, New Mexico 87185-0754, USA.
authors.forename: Jeffery A
authors.initials: JA
authors.lastname: Greathouse
authors.affiliation: Geochemistry Department, Sandia National Laboratories, Albuquerque, New Mexico 87185-0754, USA.
authors.forename: David B
authors.initials: DB
authors.lastname: Hart
authors.affiliation: Nanoscale Sciences Department, Sandia National Laboratories, Albuquerque, New Mexico 87185-1415, USA.
authors.forename: Dorina F Sava
authors.initials: DF
authors.lastname: Gallis
authors.affiliation: Physical Chemical and Nano Sciences Center, Sandia National Laboratories, Albuquerque, New Mexico 87185-1415, USA. tmnenof@sandia.gov.
authors.forename: Tina M
authors.initials: TM
authors.lastname: Nenoff