Modeling adsorption in metal-organic frameworks with open metal sites : propane/propylene separations

Fischer, Michael and Gomes, Jose R. B. and Froba, Michael and Jorge, Miguel (2012) Modeling adsorption in metal-organic frameworks with open metal sites : propane/propylene separations. Langmuir, 28 (22). pp. 8537-8549. ISSN 0743-7463 (https://doi.org/10.1021/la301215y)

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Abstract

We present a new approach for modeling adsorption in metal-organic frameworks (MOFs) with unsaturated metal centers and apply it to the challenging propane/propylene separation in copper(II) benzene-1,3,5-tricarboxylate (CuBTC). We obtain information about the specific interactions between olefins and the open metal sites of the MOP using quantum mechanical density functional theory. A proper consideration of all the relevant contributions to the adsorption energy enables us to extract the component that is due to specific attractive interactions between the pi-orbitals of the alkene and the coordinatively unsaturated metal. This component is fitted using a combination of a Morse potential and a power law function and is then included into classical grand canonical Monte Carlo simulations of adsorption. Using this modified potential model, together with a standard Lennard-Jones model, we are able to predict the adsorption of not only propane (where no specific interactions are present), but also of propylene (where specific interactions are dominant). Binary adsorption isotherms for this mixture are in reasonable agreement with ideal adsorbed solution theory predictions. We compare our approach with previous attempts to predict adsorption in MOFs with open metal sites and suggest possible future routes for improving our model.

ORCID iDs

Fischer, Michael, Gomes, Jose R. B., Froba, Michael and Jorge, Miguel ORCID logoORCID: https://orcid.org/0000-0003-3009-4725;
  • Item type:Article
    ID code:42576
    Dates:
    Date
    Event
    5 June 2012
    Published
    10 May 2012
    Published Online
    Notes:This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in Langmuir, copyright © American Chemical Society after peer review. To access the final edited and published work see http://pubs.acs.org/doi/abs/10.1021/la301215y
    Subjects:Technology > Chemical engineering
    Department:Faculty of Engineering > Chemical and Process Engineering
    Depositing user: Pure Administrator
    Date deposited:15 Jan 2013 16:13
    Last modified:11 Nov 2024 10:19
    Related URLs:
    URI:https://strathprints.strath.ac.uk/id/eprint/42576
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