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Understanding intrinsic light absorption properties of UiO-66 frameworks: a combined theoretical and experimental study

Kevin Hendrickx UGent, Danny Vanpoucke, Karen Leus UGent, Kurt Lejaeghere UGent, Andy Van Yperen-De Deyne, Veronique Van Speybroeck UGent, Pascal Van Der Voort UGent and Karen Hemelsoet UGent (2015) INORGANIC CHEMISTRY. 54(22). p.10701-10710
abstract
A combined theoretical and experimental study is performed in order to elucidate the effects of linker functional groups on the photoabsorption properties of UiO-66-X materials. This study, in which both mono- and difunctionalized linkers (with X = OH, NH2, or SH) are investigated, aims to obtain a more complete picture of the choice of functionalization. Static time-dependent density functional theory calculations combined with molecular dynamics simulations are performed on the linkers, and the results are compared to experimental UV/vis spectra in order to understand the electronic effects governing the absorption spectra. The disubstituted linkers show larger shifts than the monosubstituted variants, making them promising candidates for further study as photocatalysts. Next, the interaction between the linker and the inorganic part of the framework is theoretically investigated using a cluster model. The proposed ligand-to-metal-charge transfer is theoretically observed and is influenced by the differences in fundtionalization. Finally, the computed electronic properties of the periodic UiO-66 materials reveal that the band gap can be altered by linker functionalization and ranges from 4.0 down to 2.2 eV. Study of the periodic density of states allows the band gap modulations of the framework to be explained in terms of a functionalization-induced band in the band gap of the original UiO-66 host.
Please use this url to cite or link to this publication:
author
organization
year
type
journalArticle (original)
publication status
published
subject
keyword
METAL-ORGANIC FRAMEWORKS, DENSITY-FUNCTIONAL THEORY, BASIS-SET, ENERGY, PERIODIC MATERIALS, DRIVEN PHOTOCATALYST, ADSORPTION PROPERTIES, PHOTOCATALYTIC CO2 REDUCTION, EXTENDING HIRSHFELD-I, SEMICONDUCTOR PHOTOCATALYSIS
journal title
INORGANIC CHEMISTRY
Inorg. Chem.
volume
54
issue
22
pages
10701 - 10710
Web of Science type
Article
Web of Science id
000364981300025
JCR category
CHEMISTRY, INORGANIC & NUCLEAR
JCR impact factor
4.82 (2015)
JCR rank
4/46 (2015)
JCR quartile
1 (2015)
ISSN
0020-1669
DOI
10.1021/acs.inorgchem.5b01593
language
English
UGent publication?
yes
classification
A1
copyright statement
I have transferred the copyright for this publication to the publisher
id
7024359
handle
http://hdl.handle.net/1854/LU-7024359
date created
2016-01-05 09:16:09
date last changed
2016-12-19 15:47:04
@article{7024359,
  abstract     = {A combined theoretical and experimental study is performed in order to elucidate the effects of linker functional groups on the photoabsorption properties of UiO-66-X materials. This study, in which both mono- and difunctionalized linkers (with X = OH, NH2, or SH) are investigated, aims to obtain a more complete picture of the choice of functionalization. Static time-dependent density functional theory calculations combined with molecular dynamics simulations are performed on the linkers, and the results are compared to experimental UV/vis spectra in order to understand the electronic effects governing the absorption spectra. The disubstituted linkers show larger shifts than the monosubstituted variants, making them promising candidates for further study as photocatalysts. Next, the interaction between the linker and the inorganic part of the framework is theoretically investigated using a cluster model. The proposed ligand-to-metal-charge transfer is theoretically observed and is influenced by the differences in fundtionalization. Finally, the computed electronic properties of the periodic UiO-66 materials reveal that the band gap can be altered by linker functionalization and ranges from 4.0 down to 2.2 eV. Study of the periodic density of states allows the band gap modulations of the framework to be explained in terms of a functionalization-induced band in the band gap of the original UiO-66 host.},
  author       = {Hendrickx, Kevin and Vanpoucke, Danny and Leus, Karen and Lejaeghere, Kurt and Van Yperen-De Deyne, Andy and Van Speybroeck, Veronique and Van Der Voort, Pascal and Hemelsoet, Karen},
  issn         = {0020-1669},
  journal      = {INORGANIC CHEMISTRY},
  keyword      = {METAL-ORGANIC FRAMEWORKS,DENSITY-FUNCTIONAL THEORY,BASIS-SET,ENERGY,PERIODIC MATERIALS,DRIVEN PHOTOCATALYST,ADSORPTION PROPERTIES,PHOTOCATALYTIC CO2 REDUCTION,EXTENDING HIRSHFELD-I,SEMICONDUCTOR PHOTOCATALYSIS},
  language     = {eng},
  number       = {22},
  pages        = {10701--10710},
  title        = {Understanding intrinsic light absorption properties of UiO-66 frameworks: a combined theoretical and experimental study},
  url          = {http://dx.doi.org/10.1021/acs.inorgchem.5b01593},
  volume       = {54},
  year         = {2015},
}

Chicago
Hendrickx, Kevin, Danny Vanpoucke, Karen Leus, Kurt Lejaeghere, Andy Van Yperen-De Deyne, Veronique Van Speybroeck, Pascal Van Der Voort, and Karen Hemelsoet. 2015. “Understanding Intrinsic Light Absorption Properties of UiO-66 Frameworks: a Combined Theoretical and Experimental Study.” Inorganic Chemistry 54 (22): 10701–10710.
APA
Hendrickx, Kevin, Vanpoucke, D., Leus, K., Lejaeghere, K., Van Yperen-De Deyne, A., Van Speybroeck, V., Van Der Voort, P., et al. (2015). Understanding intrinsic light absorption properties of UiO-66 frameworks: a combined theoretical and experimental study. INORGANIC CHEMISTRY, 54(22), 10701–10710.
Vancouver
1.
Hendrickx K, Vanpoucke D, Leus K, Lejaeghere K, Van Yperen-De Deyne A, Van Speybroeck V, et al. Understanding intrinsic light absorption properties of UiO-66 frameworks: a combined theoretical and experimental study. INORGANIC CHEMISTRY. 2015;54(22):10701–10.
MLA
Hendrickx, Kevin, Danny Vanpoucke, Karen Leus, et al. “Understanding Intrinsic Light Absorption Properties of UiO-66 Frameworks: a Combined Theoretical and Experimental Study.” INORGANIC CHEMISTRY 54.22 (2015): 10701–10710. Print.