We present an entirely ab initio methodology, based on symmetry adapted perturbation theory (SAPT), for constructing force-fields to study CO2 adsorption in nanoporous zeolitic imidazolate frameworks (ZIFs). Our approach utilizes the SAPT energy decomposition to generate physically-motivated force fields for the CO2-CO2 and CO2-ZIF interaction, with explicit terms representing exchange, electrostatic, induction and dispersion interactions.  Each of these terms is fit to the corresponding term in the SAPT energy decomposition, yielding a force field almost entirely free of empirical parameters. Furthermore, the explicit correspondence between force field terms and fundamental interaction types (dispersion, electrostatics, induction) allows for an analysis of the underlying physics controlling ZIF gas absorption that is not possible with the generic force fields that had been previously utilized to study these systems. As our force fields are essentially free from empirical parameters, these results demonstrate the potential for computationally screening novel ZIFs for flue gas separation applications with near quantitative accuracy.

Ab initio, physically-motivated force fields for CO<sub>2</sub> adsorption in nanoporous solids

243rd National Meeting (2012)

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Ab initio, physically-motivated force fields for CO2 adsorption in nanoporous solids

Ab initio, physically-motivated force fields for CO₂ adsorption in nanoporous solids