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Missing linkers : an alternative pathway to UiO-66 electronic structure engineering

(2017) CHEMISTRY OF MATERIALS. 29(7). p.3006-3019
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Abstract
UiO-66 is a promising metal-organic framework for photocatalytic applications. However, the ligand-to-metal charge transfer of an excited electron is inefficient in the pristine material. Herein, we assess the influence of missing linker defects on the electronic structure of UiO-66 and discuss their ability to improve ligand-to-metal charge transfer. Using a new defect classification system, which is transparent and easily extendable, we identify the most promising photocatalysts by considering both relative stability and electronic structure. We find that the properties of UiO-66 defect structures largely depend on the coordination of the constituent nodes and that the nodes with the strongest local distortions alter the electronic structure most. Defects hence provide an alternative pathway to tune UiO-66 for photocatalytic purposes, besides linker modification and node metal substitution. In addition, the decomposition of MOF properties into node- and linker-based behavior is more generally valid, so we propose orthogonal electronic structure tuning as a paradigm in MOF design.
Keywords
METAL-ORGANIC FRAMEWORKS, PHOTOCATALYTIC CO2 REDUCTION, INITIO MOLECULAR-DYNAMICS, TOTAL-ENERGY CALCULATIONS, WAVE BASIS-SET, CATALYTIC-ACTIVITY, DEFECTS, ADSORPTION, STABILITY, LIGAND

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Chicago
De Vos, Arthur, Kevin Hendrickx, Pascal Van Der Voort, Veronique Van Speybroeck, and Kurt Lejaeghere. 2017. “Missing Linkers : an Alternative Pathway to UiO-66 Electronic Structure Engineering.” Chemistry of Materials 29 (7): 3006–3019.
APA
De Vos, Arthur, Hendrickx, K., Van Der Voort, P., Van Speybroeck, V., & Lejaeghere, K. (2017). Missing linkers : an alternative pathway to UiO-66 electronic structure engineering. CHEMISTRY OF MATERIALS, 29(7), 3006–3019.
Vancouver
1.
De Vos A, Hendrickx K, Van Der Voort P, Van Speybroeck V, Lejaeghere K. Missing linkers : an alternative pathway to UiO-66 electronic structure engineering. CHEMISTRY OF MATERIALS. 2017;29(7):3006–19.
MLA
De Vos, Arthur, Kevin Hendrickx, Pascal Van Der Voort, et al. “Missing Linkers : an Alternative Pathway to UiO-66 Electronic Structure Engineering.” CHEMISTRY OF MATERIALS 29.7 (2017): 3006–3019. Print.
@article{8519705,
  abstract     = {UiO-66 is a promising metal-organic framework for photocatalytic applications. However, the ligand-to-metal charge transfer of an excited electron is inefficient in the pristine material. Herein, we assess the influence of missing linker defects on the electronic structure of UiO-66 and discuss their ability to improve ligand-to-metal charge transfer. Using a new defect classification system, which is transparent and easily extendable, we identify the most promising photocatalysts by considering both relative stability and electronic structure. We find that the properties of UiO-66 defect structures largely depend on the coordination of the constituent nodes and that the nodes with the strongest local distortions alter the electronic structure most. Defects hence provide an alternative pathway to tune UiO-66 for photocatalytic purposes, besides linker modification and node metal substitution. In addition, the decomposition of MOF properties into node- and linker-based behavior is more generally valid, so we propose orthogonal electronic structure tuning as a paradigm in MOF design.},
  author       = {De Vos, Arthur and Hendrickx, Kevin and Van Der Voort, Pascal and Van Speybroeck, Veronique and Lejaeghere, Kurt},
  issn         = {0897-4756},
  journal      = {CHEMISTRY OF MATERIALS},
  keyword      = {METAL-ORGANIC FRAMEWORKS,PHOTOCATALYTIC CO2 REDUCTION,INITIO MOLECULAR-DYNAMICS,TOTAL-ENERGY CALCULATIONS,WAVE BASIS-SET,CATALYTIC-ACTIVITY,DEFECTS,ADSORPTION,STABILITY,LIGAND},
  language     = {eng},
  number       = {7},
  pages        = {3006--3019},
  title        = {Missing linkers : an alternative pathway to UiO-66 electronic structure engineering},
  url          = {http://dx.doi.org/10.1021/acs.chemmater.6b05444},
  volume       = {29},
  year         = {2017},
}

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