CO2 Adsorption in Fe2(dobdc): A Classical Force Field Parameterized from Quantum Mechanical Calculations

被引：43

作者：

Borycz, Joshua ^{[1
,2
]}

Lin, Li-Chiang ^{[3
]}

Bloch, Eric D. ^{[4
]}

Kim, Jihan ^{[5
]}

Dzubak, Allison L. ^{[1
,2
]}

Maurice, Remi ^{[1
,2
,6
]}

Semrouni, David ^{[1
,2
]}

Lee, Kyuho ^{[3
]}

Smit, Berend ^{[3
,4
]}

Gagliardi, Laura ^{[1
,2
]}

机构：

[1] Univ Minnesota, Dept Chem, Inst Supercomp, Minneapolis, MN 55455 USA

[2] Univ Minnesota, Chem Theory Ctr, Minneapolis, MN 55455 USA

[3] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA

[4] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA

[5] Korea Adv Inst Sci & Technol, Dept Chem & Biomol Engn, Daehak Ro 305710, South Korea

[6] Univ Nantes, SUBATECH, IN2P3, EMN Nantes,UMR CNRS 6457, F-44307 Nantes 3, France

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2014年 / 118卷 / 23期

关键词：

METAL-ORGANIC FRAMEWORK; 2ND-ORDER PERTURBATION-THEORY; INITIO MOLECULAR-DYNAMICS; TOTAL-ENERGY CALCULATIONS; CARBON-DIOXIDE CAPTURE; BASIS-SETS; ELECTRONIC-STRUCTURE; MOF MATERIAL; MIXTURES; SYSTEMS;

D O I：

10.1021/jp500313j

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Carbon dioxide adsorption isotherms have been computed for the metal-organic framework (MOF) Fe-2(dobdc), where dobdc(4-) = 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 Moller-Plesset second-order perturbation theory (ROMP2) calculations have been performed to obtain interaction energy curves between a CO2 molecule and a cluster model of Fe-2(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 Fe-2(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.

引用

页码：12230 / 12240

页数：11

共 66 条

[31]

Holt A, 2009, THESIS LUND U

[32] A NEMO Potential that Includes the Dipole-Quadrupole and Quadrupole-Quadrupole Polarizability [J].

Holt, Asbjorn ;

Bostrom, Jonas ;

Karlstrom, Gunnar ;

Lindh, Roland .

JOURNAL OF COMPUTATIONAL CHEMISTRY, 2010, 31 (08) :1583-1591

[33] O2-binding to heme:: electronic structure and spectrum of oxyheme, studied by multiconfigurational methods [J].

Jensen, KP ;

Roos, BO ;

Ryde, U .

JOURNAL OF INORGANIC BIOCHEMISTRY, 2005, 99 (01) :45-54

[34] MOLCAS:: a program package for computational chemistry [J].

Karlström, G ;

Lindh, R ;

Malmqvist, PÅ ;

Roos, BO ;

Ryde, U ;

Veryazov, V ;

Widmark, PO ;

Cossi, M ;

Schimmelpfennig, B ;

Neogrady, P ;

Seijo, L .

COMPUTATIONAL MATERIALS SCIENCE, 2003, 28 (02) :222-239

[35] AB-INITIO MOLECULAR-DYNAMICS SIMULATION OF THE LIQUID-METAL AMORPHOUS-SEMICONDUCTOR TRANSITION IN GERMANIUM [J].

KRESSE, G ;

HAFNER, J .

PHYSICAL REVIEW B, 1994, 49 (20) :14251-14269

[36] Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set [J].

Kresse, G ;

Furthmuller, J .

PHYSICAL REVIEW B, 1996, 54 (16) :11169-11186

[37] ABINITIO MOLECULAR-DYNAMICS FOR LIQUID-METALS [J].

KRESSE, G ;

HAFNER, J .

PHYSICAL REVIEW B, 1993, 47 (01) :558-561

[38] From ultrasoft pseudopotentials to the projector augmented-wave method [J].

Kresse, G ;

Joubert, D .

PHYSICAL REVIEW B, 1999, 59 (03) :1758-1775

[39] Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set [J].

Kresse, G ;

Furthmuller, J .

COMPUTATIONAL MATERIALS SCIENCE, 1996, 6 (01) :15-50

[40] A Microporous Copper Metal-Organic Framework with High H2 and CO2 Adsorption Capacity at Ambient Pressure [J].

Laessig, Daniel ;

Lincke, Joerg ;

Moellmer, Jens ;

Reichenbach, Christian ;

Moeller, Andreas ;

Glaeser, Roger ;

Kalies, Grit ;

Cychosz, Katie A. ;

Thommes, Matthias ;

Staudt, Reiner ;

Krautscheid, Harald .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2011, 50 (44) :10344-10348

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