期刊
JOURNAL OF CATALYSIS
卷 311, 期 -, 页码 114-120出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2013.11.006
关键词
Metal-organic framework; Lewis acidity; Isomerization of alpha-pinene oxide; Campholenic aldehyde
资金
- SB RAS Project [V.44.2.12]
- Federal Program Scientific and Educational Cadres of Russia [2012-1.5-12-000-1013-002]
- Basic Science Research Program through the National Research Foundation of Korea (NRF)
- Korea government (MSIP) [2013R1A2A2A01007176]
The catalytic performance of porous metal-benzenetricarboxylates, such as MIL-100(Al, Fe and Cr), MIL-110(Al) and MIL-96(Al), was investigated with a combination of physicochemical and catalytic approaches in the rearrangement of alpha-pinene oxide to campholenic aldehyde (CA). The investigation of Lewis acidity was done by EPR and IR spectroscopy using 2,2',6,6'-tetramethyl-1-piperidinyoxyl radical and benzonitrile as the probe molecules, respectively. For Al-BTCs, both these methods showed a decrease in the amount of Lewis acid sites as follows: MIL-100 > MIL-110 > MIL-96. The reaction rate and selectivity toward CA also decreased in the same order. A relatively good correlation between selectivity toward CA and the electronegativity of the metal ion was found for isostructural MIL-100(Al, Fe and Cr). The selectivity toward CA decreased in the order: MIL-100(Al) > MIL-100(Fe) > MIL-100(Cr). The high selectivity toward CA in the presence of MIL-100 has been suggested to originate from the unique structure of this material, which favors shape selectivity. (C) 2013 Elsevier Inc. All rights reserved.
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