Witman, MatthewWright, BradleySmit, Berend2019-10-242019-10-242019-10-242019-10-0310.1021/acs.jpclett.9b02449https://infoscience.epfl.ch/handle/20.500.14299/162294WOS:000489189500039A novel computational procedure, based on the principles of flat-histogram Monte Carlo, is developed for facile prediction of the adsorption thermodynamics of intrinsically flexible adsorbents. We then demonstrate how an accurate prediction of methane deliverable capacity in a metal-organic framework (MOF) with significant intrinsic flexibility requires use of such a method. Dynamic side chains in the framework respond to methane adsorbates and reorganize to exhibit a more conducive pore space at high adsorbate densities while simultaneously providing a less conducive pore space at low adsorbate densities. This "responsive pore" MOF achieves similar to 20% higher deliverable capacity than if the framework were rigid and elucidates a strategy for designing high deliverable capacity MOFs in the future.Chemistry, PhysicalNanoscience & NanotechnologyMaterials Science, MultidisciplinaryPhysics, Atomic, Molecular & ChemicalChemistryScience & Technology - Other TopicsMaterials SciencePhysicsmetal-organic frameworksmonte-carlo simulationsstructural transitionsphase-equilibriagas-adsorptionside-chainsforce-fieldthermodynamicsflexibilityalgorithmstext::journal::journal article::research article