期刊
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
卷 -, 期 23, 页码 3904-3912出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/ejic.201500299
关键词
Metal-organic frameworks; Nanoparticles; Heterogeneous catalysis; Hydrogenation; Palladium; Chemical vapor infiltration
资金
- Consolider-Ingenio (project MULTICAT)
- Severo Ochoa program
- Spanish Ministry of Science and Innovation [MAT2011-29020-C02-01]
- Cluster of Excellence RESOLV - German Deutsche Forschungsgemeinschaft (DFG) [EXC 1069]
- European Union's Horizon research and innovation programme under the Marie Skolodowska-Curie grant agreement [641887]
Host-guest inclusion properties of UiO-66 and UiO-67 metal-organic frameworks have been studied using ferrocene (FeCp2) as probe molecule. According to variable-temperature solid-state H-1 and C-13 CP-MAS-NMR, two different environments exist for adsorbed FeCp2 inside UiO-66 and UiO-67, which have been assigned to octahedral and tetrahedral cavities. At room temperature, a rapid exchange between these two adsorption sites occurs in UiO-67, while at -80 degrees C the intracrystalline traffic of FeCp2 through the triangular windows is largely hindered. In UiO-66, FeCp2 diffusion is already impeded at room temperature, in agreement with the smaller pore windows. Palladium nanoparticles (Pd NPs) encapsulated inside UiO-66 and UiO-67 have been prepared by chemical vapor infiltration of (allyl)Pd(Cp) followed by UV light irradiation. Infiltration must be carried out at low temperature (-10 degrees C) to avoid uncontrolled decomposition of the organometallic precursor and formation of Pd NPs at the external surface of the MOF. The resulting Pd-MOFs are shape selective catalysts, as shown for the hydrogenation of carbonyl compounds with different steric hindrance.
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