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Sensing the framework state and guest molecules in MIL-53(Al) via the electron paramagnetic resonance spectrum of V-IV dopant ions

Irena Nevjestic UGent, Hannes Depauw UGent, Peter Gast, Pieter Tack UGent, Davy Deduytsche UGent, Karen Leus UGent, Melissa Van Landeghem, Etienne Goovaerts, Laszlo Vincze UGent, Christophe Detavernier UGent, et al. (2017) PHYSICAL CHEMISTRY CHEMICAL PHYSICS. 19(36). p.24545-24554
abstract
X-ray diffraction (XRD) and electron paramagnetic resonance spectroscopy (EPR) were combined to study the structural transformations induced by temperature, pressure and air humidity of the "breathing'' metalorganic framework (MOF) MIL-53(Al), doped with paramagnetic V-IV ions, after activation. The correlation between in situ XRD and thermogravimetric analysis measurements showed that upon heating this MOF in air, starting from ambient temperature and pressure, the narrow pore framework first dehydrates and after that makes the transition to a large pore state (lp). The EPR spectra of V-IV=O molecular ions, replacing Al-OH in the structure, also allow to distinguish the as synthesized, hydrated (np-h) and dehydrated narrow pore (np-d), and lp states of MIL-53(Al). A careful analysis of EPR spectra recorded at microwave frequencies between 9.5 and 275 GHz demonstrates that all V-IV=O in the np-d and lp states are equivalent, whereas in the np-h state (at least two) slightly different V-IV=O sites exist. Moreover, the lp MIL-53(Al) framework is accessible to oxygen, leading to a notable broadening of the V-IV=O EPR spectrum at pressures of a few mbar, while such effect is absent for the np-h and np-d states for pressures up to 1 bar.
Please use this url to cite or link to this publication:
author
organization
year
type
journalArticle (original)
publication status
published
subject
keyword
METAL-ORGANIC FRAMEWORK, IN-VIVO, EPR, ADSORPTION, OXIMETRY, SENSORS
journal title
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Phys. Chem. Chem. Phys.
volume
19
issue
36
pages
24545 - 24554
Web of Science type
Article
Web of Science id
000411606200018
ISSN
1463-9076
1463-9084
DOI
10.1039/c7cp04760f
language
English
UGent publication?
yes
classification
A1
copyright statement
I have transferred the copyright for this publication to the publisher
id
8534452
handle
http://hdl.handle.net/1854/LU-8534452
date created
2017-10-16 12:14:53
date last changed
2017-11-09 09:47:30
@article{8534452,
  abstract     = {X-ray diffraction (XRD) and electron paramagnetic resonance spectroscopy (EPR) were combined to study the structural transformations induced by temperature, pressure and air humidity of the {\textacutedbl}breathing'' metalorganic framework (MOF) MIL-53(Al), doped with paramagnetic V-IV ions, after activation. The correlation between in situ XRD and thermogravimetric analysis measurements showed that upon heating this MOF in air, starting from ambient temperature and pressure, the narrow pore framework first dehydrates and after that makes the transition to a large pore state (lp). The EPR spectra of V-IV=O molecular ions, replacing Al-OH in the structure, also allow to distinguish the as synthesized, hydrated (np-h) and dehydrated narrow pore (np-d), and lp states of MIL-53(Al). A careful analysis of EPR spectra recorded at microwave frequencies between 9.5 and 275 GHz demonstrates that all V-IV=O in the np-d and lp states are equivalent, whereas in the np-h state (at least two) slightly different V-IV=O sites exist. Moreover, the lp MIL-53(Al) framework is accessible to oxygen, leading to a notable broadening of the V-IV=O EPR spectrum at pressures of a few mbar, while such effect is absent for the np-h and np-d states for pressures up to 1 bar.},
  author       = {Nevjestic, Irena and Depauw, Hannes and Gast, Peter and Tack, Pieter and Deduytsche, Davy and Leus, Karen and Van Landeghem, Melissa and Goovaerts, Etienne and Vincze, Laszlo and Detavernier, Christophe and Van Der Voort, Pascal and Callens, Freddy and Vrielinck, Henk},
  issn         = {1463-9076},
  journal      = {PHYSICAL CHEMISTRY CHEMICAL PHYSICS},
  keyword      = {METAL-ORGANIC FRAMEWORK,IN-VIVO,EPR,ADSORPTION,OXIMETRY,SENSORS},
  language     = {eng},
  number       = {36},
  pages        = {24545--24554},
  title        = {Sensing the framework state and guest molecules in MIL-53(Al) via the electron paramagnetic resonance spectrum of V-IV dopant ions},
  url          = {http://dx.doi.org/10.1039/c7cp04760f},
  volume       = {19},
  year         = {2017},
}

Chicago
Nevjestic, Irena, Hannes Depauw, Peter Gast, Pieter Tack, Davy Deduytsche, Karen Leus, Melissa Van Landeghem, et al. 2017. “Sensing the Framework State and Guest Molecules in MIL-53(Al) via the Electron Paramagnetic Resonance Spectrum of V-IV Dopant Ions.” Physical Chemistry Chemical Physics 19 (36): 24545–24554.
APA
Nevjestic, I., Depauw, H., Gast, P., Tack, P., Deduytsche, D., Leus, K., Van Landeghem, M., et al. (2017). Sensing the framework state and guest molecules in MIL-53(Al) via the electron paramagnetic resonance spectrum of V-IV dopant ions. PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 19(36), 24545–24554.
Vancouver
1.
Nevjestic I, Depauw H, Gast P, Tack P, Deduytsche D, Leus K, et al. Sensing the framework state and guest molecules in MIL-53(Al) via the electron paramagnetic resonance spectrum of V-IV dopant ions. PHYSICAL CHEMISTRY CHEMICAL PHYSICS. 2017;19(36):24545–54.
MLA
Nevjestic, Irena, Hannes Depauw, Peter Gast, et al. “Sensing the Framework State and Guest Molecules in MIL-53(Al) via the Electron Paramagnetic Resonance Spectrum of V-IV Dopant Ions.” PHYSICAL CHEMISTRY CHEMICAL PHYSICS 19.36 (2017): 24545–24554. Print.