期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 114, 期 39, 页码 16596-16602出版社
AMER CHEMICAL SOC
DOI: 10.1021/jp105700b
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资金
- Deutsche Forschungsgemeinschaft
- Fonds der Chemischen Industrie
H-1 and Al-27 MAS NMR spectroscopies have been applied for studying the effect of water molecules, nitrogen bases, and o-xylene on the hydroxyl protons of bridging AlOH groups and framework aluminum atoms in the metal-organic framework (MOF) MIL-53. For water molecules adsorbed on the low-temperature form MIL-53lt, two H-1 MAS NMR signals were found indicating the formation of different O-H center dot center dot center dot O hydrogen bonds to neighboring oxygen atoms, such as to carboxylic oxygens. Upon adsorption of the nitrogen bases acetonitrile, ammonia, and pyridine, a linear increase of the quadrupole coupling constant, C-Q, of the framework aluminum atoms in dehydrated MIL-53 from C-Q = 8.5 MHz (unloaded material) to maximum 10.8 MHz (pyridine-loaded material) as a function of the proton affinity of the adsorbates was observed. Adsorption of o-xylene led to three stepwise changes of the quadrupole coupling constants, C-Q of framework aluminum atoms in dehydrated MIL-53. While the first two stepwise changes of the C-Q values (C-Q = 8.0 and 8.7 MHz) occur for o-xylene loadings of lower than 4 molecules per unit cell and for all AlO4(OH)(2) centers, the third change of the C-Q value to 9.4 MHz was observed for o-xylene loadings higher than 4 o-xylene molecules per unit cell and for maximum 50% of the framework aluminum atoms. This third adsorbate-induced change of the C-Q value of framework aluminum atoms in MIL-53 is accompanied by a significant decrease of the adsorbate mobility.
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