期刊
CHEMICAL ENGINEERING JOURNAL
卷 269, 期 -, 页码 236-244出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2015.01.092
关键词
Metal-organic frameworks; MIL-100(Fe); Heterogeneous catalysis; 12-Tungstophosphoric acid; Esterification; Acetalization
资金
- Zhejiang Provincial Natural Science Foundation of China [LY13B030002]
- National Natural Science Foundation of China [20806075]
- Open Research Fund of Top Key Discipline of Chemistry in Zhejiang Provincial Colleges
- Key Laboratory of the Ministry of Education for Advanced Catalysis Materials (Zhejiang Normal University) [ZJHX201404]
12-Tungstophosphoric heteropolyacid (HPW) has been encapsulated in a mesoporous metal-organic framework (MOF), MIL-100(Fe), by a simple low-temperature (<100 degrees C) HF-free incorporation route via the reaction of ferric nitrate and trimesic acid in the presence of HPW. The resulting hybrid HPW@MIL-100(Fe) material was systemically characterized by XRD, N-2 adsorption, FT-IR, acid-base titration, P-31 MAS NMR, TEM, SEM, TGA, XPS techniques and elemental analysis, and then used as a heterogeneous catalyst in acid-catalyzed esterification and acetalization. The characterization results indicate that the HPW molecules were successfully incorporated within the mesoporous cages of the MIL-100(Fe) matrix as noncoordinating guests, thus maintaining the integrity of the protonic acidity of HPW. The resulting HPW@MIL-100(Fe) catalyst exhibits high activity and excellent reusability in the esterification reactions with no evidence for agglomeration, leaching, or deactivation of the HPW during several repeated uses of the catalyst. Similarly, the HPW@MIL-100(Fe) catalyst also shows excellent catalytic properties in the acetalization of benzaldehyde and ethanediol. The unique characteristics of MIL-100(Fe) and the uniform dispersion of HPW molecules within the mesoporous cages of the MIL-100(Fe) matrix may account for the high catalytic activity and recyclability of the HPW@MIL-100(Fe) catalyst. (C) 2015 Elsevier B.V. All rights reserved.
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