American Chemical Society
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CO2 Adsorption in Fe2(dobdc): A Classical Force Field Parameterized from Quantum Mechanical Calculations

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journal contribution
posted on 2014-06-12, 00:00 authored by Joshua Borycz, Li-Chiang Lin, Eric D. Bloch, Jihan Kim, Allison L. Dzubak, Rémi Maurice, David Semrouni, Kyuho Lee, Berend Smit, Laura Gagliardi
Carbon dioxide adsorption isotherms have been computed for the metal–organic framework (MOF) Fe2(dobdc), where dobdc4– = 2,5-dioxido-1,4-benzenedicarboxylate. A force field derived from quantum mechanical calculations has been used to model adsorption isotherms within a MOF. Restricted open-shell Møller–Plesset second-order perturbation theory (ROMP2) calculations have been performed to obtain interaction energy curves between a CO2 molecule and a cluster model of Fe2(dobdc). The force field parameters have been optimized to best reproduced these curves and used in Monte Carlo simulations to obtain CO2 adsorption isotherms. The experimental loading of CO2 adsorbed within Fe2(dobdc) was reproduced quite accurately. This parametrization scheme could easily be utilized to predict isotherms of various guests inside this and other similar MOFs not yet synthesized.