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The incorporation of coordinatively unsatd. metal sites (cus's), also known as open metal sites, into metal-org. frameworks (MOFs), significantly enhances the uptake of certain gases, such as CO2 and CH4, esp. at low loadings when fluid-framework interactions play the predominant role. However, due to the considerably enhanced, localized guest interactions with the cus's, it remains a challenge to predict correctly adsorption isotherms and mechanisms in MOFs with cus's using grand-canonical Monte Carlo (GCMC) simulations based on generic classical force fields. To address this problem, the authors carefully studied several well-established semiempirical model potentials and used a multiobjective genetic algorithm to parametrize them using accurate ab initio data as ref. The Carra-Konowalow potential, a modified Buckingham potential, in combination with the MMSV potential for the cus's gives not only adsorption isotherms in very good agreement with expts. but also correctly captures the adsorption mechanisms, including adsorption on the cus's, for CO2 in CPO-27-Mg and CH4 in CuBTC. Also, the parameters obtained also give quant. predictions of CH4 adsorption in PCN-14, another MOF with Cu cus's, which is an important step for developing transferable force fields that reliably predict adsorption in MOFs with cus's.
|Journal||Journal of Physical Chemistry C|
|Publication status||Published - 2012|
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