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Semi-analytical mean-field model for predicting breathing in metal–organic frameworks

Louis Vanduyfhuys (UGent) , An Ghysels (UGent) , Sven Rogge (UGent) , Ruben Demuynck (UGent) and Veronique Van Speybroeck (UGent)
(2015) MOLECULAR SIMULATION. 41(16-17). p.1311-1328
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Abstract
A new semi-analytical mean-field model is proposed to rationalise breathing of MIL-53 type materials. The model is applied on two case studies, the guest-induced breathing of MIL-53(Cr) with CO2 and CH4, and the phase transformations for MIL-53(Al) upon xenon adsorption. Experimentally, MIL-53(Cr) breathes upon CO2 adsorption, which was not observed for CH4. This result could be ascribed to the stronger interaction of carbon dioxide with the host matrix. For MIL-53(Al) a phase transition from the large pore phase could be enforced to an intermediate phase with volumes of about 1160–1300 Å3, which corresponds well to the phase observed experimentally upon xenon adsorption. Our thermodynamic model correlates nicely with the adsorption pressure model proposed by Coudert et al. Furthermore the model can predict breathing behaviour of other flexible materials, if the user can determine the free energy of the empty host, the interaction energy between a guest molecule and the host matrix and the pore volume accessible to the guest molecules. This will allow to generate the osmotic potential from which the equilibria can be deduced and the anticipated experimentally observed phase may be predicted.
Keywords
FORCE-FIELD, INDUCED STRUCTURAL TRANSITIONS, MIL-53, TEMPERATURE, ADSORPTION, THERMODYNAMICS, DYNAMICS, thermodynamic model, osmotic ensemble, breathing, flexible frameworks, metal-organic frameworks

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Citation

Please use this url to cite or link to this publication:

Chicago
Vanduyfhuys, Louis, An Ghysels, Sven Rogge, Ruben Demuynck, and Veronique Van Speybroeck. 2015. “Semi-analytical Mean-field Model for Predicting Breathing in Metal–organic Frameworks.” Molecular Simulation 41 (16-17): 1311–1328.
APA
Vanduyfhuys, L., Ghysels, A., Rogge, S., Demuynck, R., & Van Speybroeck, V. (2015). Semi-analytical mean-field model for predicting breathing in metal–organic frameworks. MOLECULAR SIMULATION, 41(16-17), 1311–1328.
Vancouver
1.
Vanduyfhuys L, Ghysels A, Rogge S, Demuynck R, Van Speybroeck V. Semi-analytical mean-field model for predicting breathing in metal–organic frameworks. MOLECULAR SIMULATION. Taylor & Francis; 2015;41(16-17):1311–28.
MLA
Vanduyfhuys, Louis, An Ghysels, Sven Rogge, et al. “Semi-analytical Mean-field Model for Predicting Breathing in Metal–organic Frameworks.” MOLECULAR SIMULATION 41.16-17 (2015): 1311–1328. Print.
@article{7023569,
  abstract     = {A new semi-analytical mean-field model is proposed to rationalise breathing of MIL-53 type materials. The model is applied on two case studies, the guest-induced breathing of MIL-53(Cr) with CO2 and CH4, and the phase transformations for MIL-53(Al) upon xenon adsorption. Experimentally, MIL-53(Cr) breathes upon CO2 adsorption, which was not observed for CH4. This result could be ascribed to the stronger interaction of carbon dioxide with the host matrix. For MIL-53(Al) a phase transition from the large pore phase could be enforced to an intermediate phase with volumes of about 1160--1300 {\AA}3, which corresponds well to the phase observed experimentally upon xenon adsorption. Our thermodynamic model correlates nicely with the adsorption pressure model proposed by Coudert et al. Furthermore the model can predict breathing behaviour of other flexible materials, if the user can determine the free energy of the empty host, the interaction energy between a guest molecule and the host matrix and the pore volume accessible to the guest molecules. This will allow to generate the osmotic potential from which the equilibria can be deduced and the anticipated experimentally observed phase may be predicted.},
  author       = {Vanduyfhuys, Louis and Ghysels, An and Rogge, Sven and Demuynck, Ruben and Van Speybroeck, Veronique},
  issn         = {0892-7022},
  journal      = {MOLECULAR SIMULATION},
  keyword      = {FORCE-FIELD,INDUCED STRUCTURAL TRANSITIONS,MIL-53,TEMPERATURE,ADSORPTION,THERMODYNAMICS,DYNAMICS,thermodynamic model,osmotic ensemble,breathing,flexible frameworks,metal-organic frameworks},
  language     = {eng},
  number       = {16-17},
  pages        = {1311--1328},
  publisher    = {Taylor \& Francis},
  title        = {Semi-analytical mean-field model for predicting breathing in metal--organic frameworks},
  url          = {http://dx.doi.org/10.1080/08927022.2015.1048512},
  volume       = {41},
  year         = {2015},
}

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