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Citation link: https://doi.org/10.26092/elib/2846

Publisher DOI: https://doi.org/10.1515/zkri-2014-1809
Fischer_Structure and bonding of water molecules_2015_published-version.pdf
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Structure and bonding of water molecules in zeolite hosts: Benchmarking plane-wave DFT against crystal structure data


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Authors: Fischer, Michael  
Abstract: 
Density-functional theory (DFT) calculations are widely employed to study the interaction of water molecules with zeolite frameworks. However, there have been only few attempts to assess whether these computations reproduce experimental structure data sufficiently well, especially with regard to the hydrogen positions of the water molecules. In this work, a detailed comparison between experimental crystal structures and DFT-optimised structures is made for six water-loaded natural zeolites. For each system, high-quality structure determinations from neutron diffraction data have been reported (bikitaite/Li–BIK, edingtonite/Ba–EDI, gismondine/Ca–GIS, scolecite/Ca–NAT, natrolite/Na–NAT, yugawaralite/Ca–YUG). Using a plane-wave DFT approach, the performance of six pure and three dispersion-corrected exchange-correlation functionals is compared, focusing on an optimisation of the atomic coordinates in a fixed unit cell (with cell parameters taken from experiment). It is found that the PBE and the PW91 functional give the smallest overall deviation between experiment and computation. Of the dispersion-corrected approaches, the PBE–TS functional exhibits the best performance. For the PBE and PBE–TS functionals, the agreement between experiment and DFT is analysed in more detail for different groups of interatomic distances. Regarding the OW–H distances in the water molecules, the DFT optimisations lead to physically realistic bond lengths. On the other hand, DFT has a systematic tendency to underestimate the length of hydrogen bonds. The cation-oxygen distances are mostly in very good agreement with experiment, although some exceptions indicate the necessity of further studies.
Keywords: Benchmarking; Computational chemistry; Density-functional theory; Water adsorption; Zeolites
Issue Date: 12-Feb-2015
Publisher: De Gruyter
Journal/Edited collection: Zeitschrift für Kristallographie - Crystalline Materials 
Issue: 5
Start page: 325
End page: 336
Volume: 230
Type: Artikel/Aufsatz
ISSN: 2194-4946
Secondary publication: yes
Document version: Published Version
DOI: 10.26092/elib/2846
URN: urn:nbn:de:gbv:46-elib77646
Institution: Universität Bremen 
Faculty: Fachbereich 05: Geowissenschaften (FB 05) 
Fachgebiet Kristallographie und Geomaterialforschung
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