(520b) A New Approach to Predict Adsorption in Metal-Organic Frameworks with Unsaturated Metal Sites
Our communication presents a generally applicable and transferable approach for incorporating specific coordination-type interactions between CUS and adsorbate molecules into standard molecular models, based on a combination of quantum mechanical calculations with classical Monte Carlo simulations. Crucially, our approach makes use of only a small number of QM calculations in the vicinity of the CUS, thus keeping computational expense low, while making use of conventional classical approaches to describe interactions away from the CUS [1, 2]. We demonstrate generality by applying our model to describe adsorption of both polar and non-polar adsorbates (paraffins, olefins, nitrogen and carbon monoxide) , and demonstrate transferability by predicting adsorption in different MOFs with the same type of metal unit (copper paddlewheel) . In all cases, excellent agreement with experimental adsorption isotherms is obtained. This means that the procedure is amenable for incorporation into large-scale screening efforts, and has the potential to greatly improve the accuracy of computational screening of MOFs for adsorption applications. Overall, our new model provides detailed insight into the molecular level adsorption mechanisms on MOFs with CUS, and constitutes a useful tool to design new materials for challenging separations.
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 Campbell, C.; Gomes, J. R. B.; Fischer, M.; Jorge, M. submitted for publication.
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