Benchmarking density functional theory predictions of framework structures and properties in a chemically diverse test set of metal–organic frameworks
Abstract
We compiled a test set of chemically and topologically diverse Metal–Organic Frameworks (MOFs) with high accuracy experimentally derived crystallographic structure data. The test set was used to benchmark the performance of Density Functional Theory (DFT) functionals (M06L, PBE, PW91, PBE-D2, PBE-D3, and vdW-DF2) for predicting lattice parameters, unit cell volume, bonded parameters and pore descriptors. On average PBE-D2, PBE-D3, and vdW-DF2 predict more accurate structures, but all functionals predicted pore diameters within 0.5 Å of the experimental diameter for every MOF in the test set. The test set was also used to assess the variance in performance of DFT functionals for elastic properties and atomic partial charges. The DFT predicted elastic properties such as minimum shear modulus and Young's modulus can differ by an average of 3 and 9 GPa for rigid MOFs such as those in the test set. Moreover, we calculated the partial charges by vdW-DF2 deviate the most from other functionals while there is no significant difference between the partial charges calculated by M06L, PBE, PW91, PBE-D2 and PBE-D3 for the MOFs in the test set. We find that while there are differences in the magnitude of the properties predicted by the various functionals, these discrepancies aremore »
- Authors:
-
- Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical & Biomolecular Engineering
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
- Publication Date:
- Research Org.:
- Univ. of Minnesota, Minneapolis, MN (United States). Nanoporous Materials Genome Center; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- OSTI Identifier:
- 1459356
- Alternate Identifier(s):
- OSTI ID: 1238732
- Grant/Contract Number:
- FG02-12ER16362; SC0008688; AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Materials Chemistry. A
- Additional Journal Information:
- Journal Volume: 3; Journal Issue: 44; Journal ID: ISSN 2050-7488
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Nazarian, Dalar, Ganesh, P., and Sholl, David S. Benchmarking density functional theory predictions of framework structures and properties in a chemically diverse test set of metal–organic frameworks. United States: N. p., 2015.
Web. doi:10.1039/C5TA03864B.
Nazarian, Dalar, Ganesh, P., & Sholl, David S. Benchmarking density functional theory predictions of framework structures and properties in a chemically diverse test set of metal–organic frameworks. United States. https://doi.org/10.1039/C5TA03864B
Nazarian, Dalar, Ganesh, P., and Sholl, David S. Wed .
"Benchmarking density functional theory predictions of framework structures and properties in a chemically diverse test set of metal–organic frameworks". United States. https://doi.org/10.1039/C5TA03864B. https://www.osti.gov/servlets/purl/1459356.
@article{osti_1459356,
title = {Benchmarking density functional theory predictions of framework structures and properties in a chemically diverse test set of metal–organic frameworks},
author = {Nazarian, Dalar and Ganesh, P. and Sholl, David S.},
abstractNote = {We compiled a test set of chemically and topologically diverse Metal–Organic Frameworks (MOFs) with high accuracy experimentally derived crystallographic structure data. The test set was used to benchmark the performance of Density Functional Theory (DFT) functionals (M06L, PBE, PW91, PBE-D2, PBE-D3, and vdW-DF2) for predicting lattice parameters, unit cell volume, bonded parameters and pore descriptors. On average PBE-D2, PBE-D3, and vdW-DF2 predict more accurate structures, but all functionals predicted pore diameters within 0.5 Å of the experimental diameter for every MOF in the test set. The test set was also used to assess the variance in performance of DFT functionals for elastic properties and atomic partial charges. The DFT predicted elastic properties such as minimum shear modulus and Young's modulus can differ by an average of 3 and 9 GPa for rigid MOFs such as those in the test set. Moreover, we calculated the partial charges by vdW-DF2 deviate the most from other functionals while there is no significant difference between the partial charges calculated by M06L, PBE, PW91, PBE-D2 and PBE-D3 for the MOFs in the test set. We find that while there are differences in the magnitude of the properties predicted by the various functionals, these discrepancies are small compared to the accuracy necessary for most practical applications.},
doi = {10.1039/C5TA03864B},
journal = {Journal of Materials Chemistry. A},
number = 44,
volume = 3,
place = {United States},
year = {Wed Sep 30 00:00:00 EDT 2015},
month = {Wed Sep 30 00:00:00 EDT 2015}
}
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