期刊
PHYSICA STATUS SOLIDI B-BASIC SOLID STATE PHYSICS
卷 249, 期 2, 页码 335-342出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/pssb.201100634
关键词
adsorption properties; density-functional theory; DFTB; metal-organic frameworks; structural properties
资金
- Bulgarian National Science Fund [DSVP 02/1, DCVP 02/2]
- Deutsche Forschungsgemeinschaft (DFG) [SPP 1362]
- European Research Council (ERC) [StG 56962]
- European Commission (HYPOMAP) [NMP3-SL-2008-233482, MC-IAPP-2009-251149]
- DAAD
- Bulgarian Supercomputer Center
Density-functional based tight-binding (DFTB) is a powerful method to describe large molecules and materials. Metal-organic frameworks (MOFs), materials with interesting catalytic properties and with very large surface areas, have been developed and have become commercially available. Unit cells of MOFs typically include hundreds of atoms, which make the application of standard density-functional methods computationally very expensive, sometimes even unfeasible. The aim of this paper is to prepare and to validate the self-consistent charge-DFTB (SCC-DFTB) method for MOFs containing Cu, Zn, and Al metal centers. The method has been validated against full hybrid density-functional calculations for model clusters, against gradient corrected density-functional calculations for supercells, and against experiment. Moreover, the modular concept of MOF chemistry has been discussed on the basis of their electronic properties. We concentrate on MOFs comprising three common connector units: copper paddlewheels (HKUST-1), zinc oxide Zn4O tetrahedron (MOF-5, MOF-177, DUT-6 (MOF-205)), and aluminum oxide AlO4(OH)(2) octahedron (MIL-53). We show that SCC-DFTB predicts structural parameters with a very good accuracy (with less than 5% deviation, even for adsorbed CO and H2O on HKUST-1), while adsorption energies differ by 12 kJ mol(-1) or less for CO and water compared to DFT benchmark calculations.
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