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Tuning the balance between dispersion and entropy to design temperature-responsive flexible metal-organic frameworks

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Abstract
Temperature-responsive flexibility in metal-organic frameworks (MOFs) appeals to the imagination. The ability to transform upon thermal stimuli while retaining a given crystalline topology is desired for specialized sensors and actuators. However, rational design of such shape-memory nanopores is hampered by a lack of knowledge on the nanoscopic interactions governing the observed behavior. Using the prototypical MIL-53(Al) as a starting point, we show that the phase transformation between a narrow-pore and large-pore phase is determined by a delicate balance between dispersion stabilization at low temperatures and entropic effects at higher ones. We present an accurate theoretical framework that allows designing breathing thermo-responsive MOFs, based on many-electron data for the dispersion interactions and density-functional theory entropy contributions. Within an isoreticular series of materials, MIL-53(Al), MIL-53(Al)-FA, DUT-4, DUT-5 and MIL-53(Ga), only MIL-53(Al) and MIL-53(Ga) are proven to switch phases within a realistic temperature range.
Keywords
General Biochemistry, Genetics and Molecular Biology, General Physics and Astronomy, General Chemistry

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

Chicago
Wieme, Jelle, Kurt Lejaeghere, Georg Kresse, and Veronique Van Speybroeck. 2018. “Tuning the Balance Between Dispersion and Entropy to Design Temperature-responsive Flexible Metal-organic Frameworks.” Nature Communications 9 (1).
APA
Wieme, J., Lejaeghere, K., Kresse, G., & Van Speybroeck, V. (2018). Tuning the balance between dispersion and entropy to design temperature-responsive flexible metal-organic frameworks. NATURE COMMUNICATIONS, 9(1).
Vancouver
1.
Wieme J, Lejaeghere K, Kresse G, Van Speybroeck V. Tuning the balance between dispersion and entropy to design temperature-responsive flexible metal-organic frameworks. NATURE COMMUNICATIONS. Springer Nature America, Inc; 2018;9(1).
MLA
Wieme, Jelle et al. “Tuning the Balance Between Dispersion and Entropy to Design Temperature-responsive Flexible Metal-organic Frameworks.” NATURE COMMUNICATIONS 9.1 (2018): n. pag. Print.
@article{8583799,
  abstract     = {Temperature-responsive flexibility in metal-organic frameworks (MOFs) appeals to the imagination. The ability to transform upon thermal stimuli while retaining a given crystalline topology is desired for specialized sensors and actuators. However, rational design of such shape-memory nanopores is hampered by a lack of knowledge on the nanoscopic interactions governing the observed behavior. Using the prototypical MIL-53(Al) as a starting point, we show that the phase transformation between a narrow-pore and large-pore phase is determined by a delicate balance between dispersion stabilization at low temperatures and entropic effects at higher ones. We present an accurate theoretical framework that allows designing breathing thermo-responsive MOFs, based on many-electron data for the dispersion interactions and density-functional theory entropy contributions. Within an isoreticular series of materials, MIL-53(Al), MIL-53(Al)-FA, DUT-4, DUT-5 and MIL-53(Ga), only MIL-53(Al) and MIL-53(Ga) are proven to switch phases within a realistic temperature range.},
  articleno    = {4899},
  author       = {Wieme, Jelle and Lejaeghere, Kurt and Kresse, Georg and Van Speybroeck, Veronique},
  issn         = {2041-1723},
  journal      = {NATURE COMMUNICATIONS},
  language     = {eng},
  number       = {1},
  publisher    = {Springer Nature America, Inc},
  title        = {Tuning the balance between dispersion and entropy to design temperature-responsive flexible metal-organic frameworks},
  url          = {http://dx.doi.org/10.1038/s41467-018-07298-4},
  volume       = {9},
  year         = {2018},
}

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