CO2 Adsorption in Fe2(dobdc): A Classical Force Field Parameterized from Quantum Mechanical Calculations
详细信息 查看全文
- 作者：Joshua Borycz ; Li-Chiang Lin ; Eric D. Bloch ; Jihan Kim ; Allison L. Dzubak ; R茅mi Maurice ; David Semrouni ; Kyuho Lee ; Berend Smit ; Laura Gagliardi
- 刊名：Journal of Physical Chemistry C
- 出版年：2014
- 出版时间：June 12, 2014
- 年：2014
- 卷：118
- 期：23
- 页码：12230-12240
- 全文大小：559K
- 年卷期：v.118,no.23(June 12, 2014)
- ISSN：1932-7455
文摘
Carbon dioxide adsorption isotherms have been computed for the metal鈥搊rganic framework (MOF) Fe2(dobdc), where dobdc4鈥?/sup> = 2,5-dioxido-1,4-benzenedicarboxylate. A force field derived from quantum mechanical calculations has been used to model adsorption isotherms within a MOF. Restricted open-shell M酶ller鈥揚lesset second-order perturbation theory (ROMP2) calculations have been performed to obtain interaction energy curves between a CO2 molecule and a cluster model of Fe2(dobdc). The force field parameters have been optimized to best reproduced these curves and used in Monte Carlo simulations to obtain CO2 adsorption isotherms. The experimental loading of CO2 adsorbed within Fe2(dobdc) was reproduced quite accurately. This parametrization scheme could easily be utilized to predict isotherms of various guests inside this and other similar MOFs not yet synthesized.