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Effect of Partial Charge Calculation Method on Adsorption Thermodynamics in Metal-organic Frameworks

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Depiction of interactions of carbon dioxide with a porous adsorbent. Credit: NIST.

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Secure.gov websites use HTTPS A lock or https:// means you’ve safely connected to the.gov website. In classical molecular simulations, electrostatic contributions to the potential energy are typically accounted for by assigning partial charges to some or all atoms in the system. The adsorption properties obtained by simulation then serve as a qualitative measure of the variability that may follow from the choice of partial charge calculation method. Electrostatic interactions are an important contribution to the interatomic or intermolecular potential energy in any system, whether homogeneous (bulk phase) or heterogeneous (fluid and confining material or multiple fluid phases). Such ab initio methods may be incorporated into molecular simulations to model complex systems, e.g., the Car-Parrinello Molecular Dynamics method, though at high computational cost. For crystalline materials, such as metal-organic frameworks (MOF), partial charges are often computed from ab initio calculations of some prescribed method.

In this project, they use a few partial charge calculation schemes to compute thermodynamic properties via Monte Carlo molecular simulations to provide some qualitative evaluation of the affect of the charge scheme on those properties.

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