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Thermodynamic insight in the high-pressure behavior of UiO-66: effect of linker defects and linker expansion

(2016) CHEMISTRY OF MATERIALS. 28(16). p.5721-5732
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Abstract
In this Article, we present a molecular-level understanding of the experimentally observed loss of crystallinity in UiO-66-type metal organic frameworks, including the pristine UiO-66 to-68 as well as defect-containing UiO-66 materials, under the influence of external pressure. This goal is achieved by constructing pressure-versus-volume profiles at finite temperatures using a thermodynamic approach relying on ab initio derived force fields. On the atomic level, the phenomenon is reflected in a sudden drop in the number of symmetry operators for the crystallographic unit cell because of the disordered displacement of the organic linkers with respect to the inorganic bricks. For the defect-containing samples, a reduced mechanical stability is observed, however, critically depending on the distribution of these defects throughout the material, hence demonstrating the importance of judiciously characterizing defects in these materials.
Keywords
METAL-ORGANIC FRAMEWORKS, CRYSTALLINE POROUS MATERIALS, ZEOLITIC IMIDAZOLATE FRAMEWORKS, MM3 FORCE-FIELD, VAN-DER-WAALS, MOLECULAR-DYNAMICS, MECHANICAL-PROPERTIES, CANONICAL ENSEMBLE, ISORETICULAR MOFS, STABILITY

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Chicago
Rogge, Sven, Jelle Wieme, Louis Vanduyfhuys, Steven Vandenbrande, Guillaume Maurin, Toon Verstraelen, Michel Waroquier, and Veronique Van Speybroeck. 2016. “Thermodynamic Insight in the High-pressure Behavior of UiO-66: Effect of Linker Defects and Linker Expansion.” Chemistry of Materials 28 (16): 5721–5732.
APA
Rogge, S., Wieme, J., Vanduyfhuys, L., Vandenbrande, S., Maurin, G., Verstraelen, T., Waroquier, M., et al. (2016). Thermodynamic insight in the high-pressure behavior of UiO-66: effect of linker defects and linker expansion. CHEMISTRY OF MATERIALS, 28(16), 5721–5732.
Vancouver
1.
Rogge S, Wieme J, Vanduyfhuys L, Vandenbrande S, Maurin G, Verstraelen T, et al. Thermodynamic insight in the high-pressure behavior of UiO-66: effect of linker defects and linker expansion. CHEMISTRY OF MATERIALS. 2016;28(16):5721–32.
MLA
Rogge, Sven, Jelle Wieme, Louis Vanduyfhuys, et al. “Thermodynamic Insight in the High-pressure Behavior of UiO-66: Effect of Linker Defects and Linker Expansion.” CHEMISTRY OF MATERIALS 28.16 (2016): 5721–5732. Print.
@article{8095503,
  abstract     = {In this Article, we present a molecular-level understanding of the experimentally observed loss of crystallinity in UiO-66-type metal organic frameworks, including the pristine UiO-66 to-68 as well as defect-containing UiO-66 materials, under the influence of external pressure. This goal is achieved by constructing pressure-versus-volume profiles at finite temperatures using a thermodynamic approach relying on ab initio derived force fields. On the atomic level, the phenomenon is reflected in a sudden drop in the number of symmetry operators for the crystallographic unit cell because of the disordered displacement of the organic linkers with respect to the inorganic bricks. For the defect-containing samples, a reduced mechanical stability is observed, however, critically depending on the distribution of these defects throughout the material, hence demonstrating the importance of judiciously characterizing defects in these materials.},
  author       = {Rogge, Sven and Wieme, Jelle and Vanduyfhuys, Louis and Vandenbrande, Steven and Maurin, Guillaume and Verstraelen, Toon and Waroquier, Michel and Van Speybroeck, Veronique},
  issn         = {0897-4756},
  journal      = {CHEMISTRY OF MATERIALS},
  keyword      = {METAL-ORGANIC FRAMEWORKS,CRYSTALLINE POROUS MATERIALS,ZEOLITIC IMIDAZOLATE FRAMEWORKS,MM3 FORCE-FIELD,VAN-DER-WAALS,MOLECULAR-DYNAMICS,MECHANICAL-PROPERTIES,CANONICAL ENSEMBLE,ISORETICULAR MOFS,STABILITY},
  language     = {eng},
  number       = {16},
  pages        = {5721--5732},
  title        = {Thermodynamic insight in the high-pressure behavior of UiO-66: effect of linker defects and linker expansion},
  url          = {http://dx.doi.org/10.1021/acs.chemmater.6b01956},
  volume       = {28},
  year         = {2016},
}

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