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Ab initio parametrized force field for the flexible metal-organic framework MIL-53(Al)

Louis Vanduyfhuys UGent, Toon Verstraelen UGent, Matthias Vandichel UGent, Michel Waroquier UGent and Veronique Van Speybroeck UGent (2012) JOURNAL OF CHEMICAL THEORY AND COMPUTATION. 8(9). p.3217-3231
abstract
A force field is proposed for the flexible metal–organic framework MIL-53(Al), which is calibrated using density functional theory calculations on nonperiodic clusters. The force field has three main contributions: an electrostatic term based on atomic charges derived with a modified Hirshfeld-I method, a van der Waals (vdW) term with parameters taken from the MM3 model, and a valence force field whose parameters were estimated with a new methodology that uses the gradients and Hessian matrix elements retrieved from nonperiodic cluster calculations. The new force field predicts geometries and cell parameters that compare well with the experimental values both for the large and narrow pore phases. The energy profile along the breathing mode of the empty material reveals the existence of two minima, which confirms the intrinsic bistable behavior of the MIL-53. Even without the stimulus of external guest molecules, the material may transform from the large pore (lp) to the narrow pore (np) phase [Liu et al. J. Am. Chem. Soc.2008, 120, 11813]. The relative stability of the two phases critically depends on the vdW parameters, and the MM3 dispersion interaction has the tendency to overstabilize the np phase.
Please use this url to cite or link to this publication:
author
organization
year
type
journalArticle (original)
publication status
published
subject
keyword
AUGMENTED-WAVE METHOD, MOLECULAR-ORBITAL METHODS, ALUMINUM TEREPHTHALATE MIL-53, GAUSSIAN-BASIS SETS, VAN-DER-WAALS, DENSITY FUNCTIONALS, CARBON-DIOXIDE, STRUCTURAL TRANSITION, COORDINATION POLYMERS, DYNAMICS SIMULATIONS
journal title
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
J. Chem. Theory Comput.
volume
8
issue
9
pages
3217 - 3231
Web of Science type
Article
Web of Science id
000308830700026
JCR category
PHYSICS, ATOMIC, MOLECULAR & CHEMICAL
JCR impact factor
5.389 (2012)
JCR rank
3/34 (2012)
JCR quartile
1 (2012)
ISSN
1549-9618
DOI
10.1021/ct300172m
language
English
UGent publication?
yes
classification
A1
copyright statement
I have transferred the copyright for this publication to the publisher
id
3062988
handle
http://hdl.handle.net/1854/LU-3062988
date created
2012-11-29 16:08:43
date last changed
2012-11-30 10:02:42
@article{3062988,
  abstract     = {A force field is proposed for the flexible metal--organic framework MIL-53(Al), which is calibrated using density functional theory calculations on nonperiodic clusters. The force field has three main contributions: an electrostatic term based on atomic charges derived with a modified Hirshfeld-I method, a van der Waals (vdW) term with parameters taken from the MM3 model, and a valence force field whose parameters were estimated with a new methodology that uses the gradients and Hessian matrix elements retrieved from nonperiodic cluster calculations. The new force field predicts geometries and cell parameters that compare well with the experimental values both for the large and narrow pore phases. The energy profile along the breathing mode of the empty material reveals the existence of two minima, which confirms the intrinsic bistable behavior of the MIL-53. Even without the stimulus of external guest molecules, the material may transform from the large pore (lp) to the narrow pore (np) phase [Liu et al. J. Am. Chem. Soc.2008, 120, 11813]. The relative stability of the two phases critically depends on the vdW parameters, and the MM3 dispersion interaction has the tendency to overstabilize the np phase.},
  author       = {Vanduyfhuys, Louis and Verstraelen, Toon and Vandichel, Matthias and Waroquier, Michel and Van Speybroeck, Veronique},
  issn         = {1549-9618},
  journal      = {JOURNAL OF CHEMICAL THEORY AND COMPUTATION},
  keyword      = {AUGMENTED-WAVE METHOD,MOLECULAR-ORBITAL METHODS,ALUMINUM TEREPHTHALATE MIL-53,GAUSSIAN-BASIS SETS,VAN-DER-WAALS,DENSITY FUNCTIONALS,CARBON-DIOXIDE,STRUCTURAL TRANSITION,COORDINATION POLYMERS,DYNAMICS SIMULATIONS},
  language     = {eng},
  number       = {9},
  pages        = {3217--3231},
  title        = {Ab initio parametrized force field for the flexible metal-organic framework MIL-53(Al)},
  url          = {http://dx.doi.org/10.1021/ct300172m},
  volume       = {8},
  year         = {2012},
}

Chicago
Vanduyfhuys, Louis, Toon Verstraelen, Matthias Vandichel, Michel Waroquier, and Veronique Van Speybroeck. 2012. “Ab Initio Parametrized Force Field for the Flexible Metal-organic Framework MIL-53(Al).” Journal of Chemical Theory and Computation 8 (9): 3217–3231.
APA
Vanduyfhuys, L., Verstraelen, T., Vandichel, M., Waroquier, M., & Van Speybroeck, V. (2012). Ab initio parametrized force field for the flexible metal-organic framework MIL-53(Al). JOURNAL OF CHEMICAL THEORY AND COMPUTATION, 8(9), 3217–3231.
Vancouver
1.
Vanduyfhuys L, Verstraelen T, Vandichel M, Waroquier M, Van Speybroeck V. Ab initio parametrized force field for the flexible metal-organic framework MIL-53(Al). JOURNAL OF CHEMICAL THEORY AND COMPUTATION. 2012;8(9):3217–31.
MLA
Vanduyfhuys, Louis, Toon Verstraelen, Matthias Vandichel, et al. “Ab Initio Parametrized Force Field for the Flexible Metal-organic Framework MIL-53(Al).” JOURNAL OF CHEMICAL THEORY AND COMPUTATION 8.9 (2012): 3217–3231. Print.