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Methane adsorption in Zr-based MOFs : comparison and critical evaluation of force fields

(2017) JOURNAL OF PHYSICAL CHEMISTRY C. 121(45). p.25309-25322
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Abstract
The search for nanoporous materials that are highly performing for gas storage and separation is one of the contemporary challenges in material design. The computational tools to aid these experimental efforts are widely available, and adsorption isotherms are routinely computed for huge sets of (hypothetical) frameworks. Clearly the computational results depend on the interactions between the adsorbed species and the adsorbent, which are commonly described using force fields. In this paper, an extensive comparison and in-depth investigation of several force fields from literature is reported for the case of methane adsorption in the Zr-based Metal-Organic Frameworks UiO-66, UiO-67, DUT-52, NU-1000, and MOF-808. Significant quantitative differences in the computed uptake are observed when comparing different force fields, but most qualitative features are common which suggests some predictive power of the simulations when it comes to these properties. More insight into the host-guest interactions is obtained by benchmarking the force fields with an extensive number of ab initio computed single molecule interaction energies. This analysis at the molecular level reveals that especially ab initio derived force fields perform well in reproducing the ab initio interaction energies. Finally, the high sensitivity of uptake predictions on the underlying potential energy surface is explored.
Keywords
METAL-ORGANIC FRAMEWORKS, TOTAL-ENERGY CALCULATIONS, WAVE BASIS-SET, GAS-ADSORPTION, MOLECULAR-MECHANICS, LINKER DEFECTS, UIO-66, SIMULATIONS, POTENTIALS, STABILITY

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MLA
Vandenbrande, Steven et al. “Methane Adsorption in Zr-based MOFs : Comparison and Critical Evaluation of Force Fields.” JOURNAL OF PHYSICAL CHEMISTRY C 121.45 (2017): 25309–25322. Print.
APA
Vandenbrande, S., Verstraelen, T., Gutiérrez Sevillano, J. J., Waroquier, M., & Van Speybroeck, V. (2017). Methane adsorption in Zr-based MOFs : comparison and critical evaluation of force fields. JOURNAL OF PHYSICAL CHEMISTRY C, 121(45), 25309–25322.
Chicago author-date
Vandenbrande, Steven, Toon Verstraelen, Juan José Gutiérrez Sevillano, Michel Waroquier, and Veronique Van Speybroeck. 2017. “Methane Adsorption in Zr-based MOFs : Comparison and Critical Evaluation of Force Fields.” Journal of Physical Chemistry C 121 (45): 25309–25322.
Chicago author-date (all authors)
Vandenbrande, Steven, Toon Verstraelen, Juan José Gutiérrez Sevillano, Michel Waroquier, and Veronique Van Speybroeck. 2017. “Methane Adsorption in Zr-based MOFs : Comparison and Critical Evaluation of Force Fields.” Journal of Physical Chemistry C 121 (45): 25309–25322.
Vancouver
1.
Vandenbrande S, Verstraelen T, Gutiérrez Sevillano JJ, Waroquier M, Van Speybroeck V. Methane adsorption in Zr-based MOFs : comparison and critical evaluation of force fields. JOURNAL OF PHYSICAL CHEMISTRY C. American Chemical Society (ACS); 2017;121(45):25309–22.
IEEE
[1]
S. Vandenbrande, T. Verstraelen, J. J. Gutiérrez Sevillano, M. Waroquier, and V. Van Speybroeck, “Methane adsorption in Zr-based MOFs : comparison and critical evaluation of force fields,” JOURNAL OF PHYSICAL CHEMISTRY C, vol. 121, no. 45, pp. 25309–25322, 2017.
@article{8545216,
  abstract     = {The search for nanoporous materials that are highly performing for gas storage and separation is one of the contemporary challenges in material design. The computational tools to aid these experimental efforts are widely available, and adsorption isotherms are routinely computed for huge sets of (hypothetical) frameworks. Clearly the computational results depend on the interactions between the adsorbed species and the adsorbent, which are commonly described using force fields. In this paper, an extensive comparison and in-depth investigation of several force fields from literature is reported for the case of methane adsorption in the Zr-based Metal-Organic Frameworks UiO-66, UiO-67, DUT-52, NU-1000, and MOF-808. Significant quantitative differences in the computed uptake are observed when comparing different force fields, but most qualitative features are common which suggests some predictive power of the simulations when it comes to these properties. More insight into the host-guest interactions is obtained by benchmarking the force fields with an extensive number of ab initio computed single molecule interaction energies. This analysis at the molecular level reveals that especially ab initio derived force fields perform well in reproducing the ab initio interaction energies. Finally, the high sensitivity of uptake predictions on the underlying potential energy surface is explored.},
  author       = {Vandenbrande, Steven and Verstraelen, Toon and Gutiérrez Sevillano, Juan José and Waroquier, Michel and Van Speybroeck, Veronique},
  issn         = {1932-7447},
  journal      = {JOURNAL OF PHYSICAL CHEMISTRY C},
  keywords     = {METAL-ORGANIC FRAMEWORKS,TOTAL-ENERGY CALCULATIONS,WAVE BASIS-SET,GAS-ADSORPTION,MOLECULAR-MECHANICS,LINKER DEFECTS,UIO-66,SIMULATIONS,POTENTIALS,STABILITY},
  language     = {eng},
  number       = {45},
  pages        = {25309--25322},
  publisher    = {American Chemical Society (ACS)},
  title        = {Methane adsorption in Zr-based MOFs : comparison and critical evaluation of force fields},
  url          = {http://dx.doi.org/10.1021/acs.jpcc.7b08971},
  volume       = {121},
  year         = {2017},
}

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