Nanoporous solids such as zeolites and metal-organic frameworks have wide applications in gas separation and storage, and have recently received attention as possible materials for efficient carbon dioxide capture. This class of materials exhibits a wide variety of pore sizes, geometries, and connectivities, as well as a range of exposed chemical species and ligands that may bind a given adsorbate more or less favorably. These variations allow enormous potential for optimizing physical properties, such as the selective adsorption of one species over another. Density functional theory (DFT) calculations assist in the rational design of new materials by providing quantitative results on the stability of the framework and the binding energies of adsorbate species. Research opportunities are available to use DFT methods on problems in nanoporous solids, including, but not limited to: (1) the thermodynamics and phase transitions of flexible nanoporous materials, (2) the preferred binding sites of adsorbate species in nanoporous solids and predicted experimental signals (e.g., infrared spectra), and (3) the development of DFT-based force field models for the high-throughput simulation of adsorption isotherms in nanoporous solids.
Cockayne E, Wong-Ng W, Chen YS, Culp JT, Allen AJ: Density Functional Theory Study of the Structure of the Pillared Hofmann Compound Ni(3-Methyl-4,4 '-bipyridine)[Ni(CN)(4)] (Ni-BpyMe or PICNIC-21). Journal of Physical Chemistry C 125:15882, 2021
Cockayne E: Thermodynamics of the Flexible Metal-Organic Framework Material MIL-53(Cr) from First Princples. Journal of Physical Chemistry C 121:4312, 2017.
Cockayne E, Nelson EB: Density functional theory meta GGA+U study of water incorporation in the metal-organic framework material Cu-BTC. Journal of Chemical Physics 143: 024701, 2015
Li L, Cockayne E, et al: First-principles studies of carbon dioxide adsorption in cryptomelane/hollandite-type manganese dioxide. Chemical Physics Letters 580: 120, 2013
Nanoporous materials; CO2 capture; Gas adsorption; Metal-organic frameworks; DFT; Theory and modeling; Computational thermodynamics;