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Bimetallic-organic framework as a zero-leaching catalyst in the aerobic oxidation of cyclohexene

Ying-Ya Liu (UGent) , Karen Leus (UGent) , Thomas Bogaerts (UGent) , Karen Hemelsoet (UGent) , Els Bruneel (UGent) , Veronique Van Speybroeck (UGent) and Pascal Van Der Voort (UGent)
(2013) CHEMCATCHEM. 5(12). p.3657-3664
Author
Organization
Project
01M00409 (Methusalem grant)
Project
240483 ERC starting grant
Project
01P02911T (Ghent University BOF Grant )
Project
01G00710 (Ghent University GOA grant)
Abstract
A gallium 2,2-bipyridine-5,5-dicarboxylate metal-organic framework (MOF), denoted as COMOC-4, has been synthesized by solvothermal synthesis. This MOF exhibits the same topology as MOF-253. CuCl2 was incorporated into COMOC-4 by a post-synthetic modification (PSM). The spectroscopic absorption properties of the MOF framework before and after PSM were compared with theoretical data obtained by employing molecular dynamics combined with time-dependent DFT calculations on both the as-synthesized and functionalized linker. The catalytic behavior of the resulting Cu2+@COMOC-4 material was evaluated in the aerobic oxidation of cyclohexene with isobutyraldehyde as a co-oxidant. In addition, the catalytic performance of Cu2+@COMOC-4 was compared with that of the commercially available Cu-BTC (BTC=benzene-1,3,5-tricarboxylate) MOF. Cu2+@COMOC-4 exhibits a good cyclohexene conversion and an excellent selectivity towards cyclohexene oxide in comparison to the Cu-based reference catalyst. Furthermore, no leaching of the active Cu sites was observed during at least four consecutive runs.
Keywords
metal-organic framework, SPACE GAUSSIAN PSEUDOPOTENTIALS, heterogeneous catalysis, epoxidation, copper, abinitio calculations, HETEROGENEOUS CATALYSIS, METAL, EPOXIDATION, OLEFINS, DENSITY, CHEMISTRY, COMPLEX, ALKENES, ALKANES

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Citation

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Chicago
Liu, Ying-Ya, Karen Leus, Thomas Bogaerts, Karen Hemelsoet, Els Bruneel, Veronique Van Speybroeck, and Pascal Van Der Voort. 2013. “Bimetallic-organic Framework as a Zero-leaching Catalyst in the Aerobic Oxidation of Cyclohexene.” Chemcatchem 5 (12): 3657–3664.
APA
Liu, Y.-Y., Leus, K., Bogaerts, T., Hemelsoet, K., Bruneel, E., Van Speybroeck, V., & Van Der Voort, P. (2013). Bimetallic-organic framework as a zero-leaching catalyst in the aerobic oxidation of cyclohexene. CHEMCATCHEM, 5(12), 3657–3664.
Vancouver
1.
Liu Y-Y, Leus K, Bogaerts T, Hemelsoet K, Bruneel E, Van Speybroeck V, et al. Bimetallic-organic framework as a zero-leaching catalyst in the aerobic oxidation of cyclohexene. CHEMCATCHEM. 2013;5(12):3657–64.
MLA
Liu, Ying-Ya, Karen Leus, Thomas Bogaerts, et al. “Bimetallic-organic Framework as a Zero-leaching Catalyst in the Aerobic Oxidation of Cyclohexene.” CHEMCATCHEM 5.12 (2013): 3657–3664. Print.
@article{4226866,
  abstract     = {A gallium 2,2-bipyridine-5,5-dicarboxylate metal-organic framework (MOF), denoted as COMOC-4, has been synthesized by solvothermal synthesis. This MOF exhibits the same topology as MOF-253. CuCl2 was incorporated into COMOC-4 by a post-synthetic modification (PSM). The spectroscopic absorption properties of the MOF framework before and after PSM were compared with theoretical data obtained by employing molecular dynamics combined with time-dependent DFT calculations on both the as-synthesized and functionalized linker. The catalytic behavior of the resulting Cu2+@COMOC-4 material was evaluated in the aerobic oxidation of cyclohexene with isobutyraldehyde as a co-oxidant. In addition, the catalytic performance of Cu2+@COMOC-4 was compared with that of the commercially available Cu-BTC (BTC=benzene-1,3,5-tricarboxylate) MOF. Cu2+@COMOC-4 exhibits a good cyclohexene conversion and an excellent selectivity towards cyclohexene oxide in comparison to the Cu-based reference catalyst. Furthermore, no leaching of the active Cu sites was observed during at least four consecutive runs.},
  author       = {Liu, Ying-Ya and Leus, Karen and Bogaerts, Thomas and Hemelsoet, Karen and Bruneel, Els and Van Speybroeck, Veronique and Van Der Voort, Pascal},
  issn         = {1867-3880},
  journal      = {CHEMCATCHEM},
  keyword      = {metal-organic framework,SPACE GAUSSIAN PSEUDOPOTENTIALS,heterogeneous catalysis,epoxidation,copper,abinitio calculations,HETEROGENEOUS CATALYSIS,METAL,EPOXIDATION,OLEFINS,DENSITY,CHEMISTRY,COMPLEX,ALKENES,ALKANES},
  language     = {eng},
  number       = {12},
  pages        = {3657--3664},
  title        = {Bimetallic-organic framework as a zero-leaching catalyst in the aerobic oxidation of cyclohexene},
  url          = {http://dx.doi.org/10.1002/cctc.201300529},
  volume       = {5},
  year         = {2013},
}

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