A Polarizable and Transferable PHAST CO2 Potential for Materials Simulation

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• 作者：Ashley L. Mullen ; Tony Pham ; Katherine A. Forrest ; Christian R. Cioce ; Keith McLaughlin ; Brian Space
• 刊名：Journal of Chemical Theory and Computation
• 出版年：2013
• 出版时间：December 10, 2013
• 年：2013
• 卷：9
• 期：12
• 页码：5421-5429
• 全文大小：519K
• 年卷期：v.9,no.12(December 10, 2013)
• ISSN：1549-9626

文摘

Reliable PHAST (Potentials with High Accuracy Speed and Transferability) intermolecular potential energy functions for CO₂ have been developed from first principles for use in heterogeneous systems, including one with explicit polarization. The intermolecular potentials have been expressed in a transferable form and parametrized from nearly exact electronic structure calculations. Models with and without explicit many-body polarization effects, known to be important in simulation of interfacial processes, are constructed. The models have been validated on pressure鈥揹ensity isotherms of bulk CO₂ and adsorption in three metal鈥搊rganic framework (MOF) materials. The present models appear to offer advantages over high quality fluid/liquid state potentials in describing CO₂ interactions in interfacial environments where sorbates adopt orientations not commonly explored in bulk fluids. Thus, the nonpolar CO₂-PHAST and polarizable CO₂-PHAST* potentials are recommended for materials/interfacial simulations.