Journal
MICROPOROUS AND MESOPOROUS MATERIALS
Volume 170, Issue -, Pages 36-44Publisher
ELSEVIER
DOI: 10.1016/j.micromeso.2012.11.021
Keywords
Metal-organic framework; MIL-101; Polyoxometalates; Host-guest; Oxidative desulfurization
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Funding
- National Basic Research Program of China [2010CB226905]
- National Natural Science Foundation, China [21176258, U1162203]
- Specialized Research Fund for the Doctoral Program of Higher Education [20110133110002]
- Fundamental Research Funds for the Central Universities [27R1104065A]
- Natural Science Foundation of Shandong Province [ZR2011BQ004]
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Successful encapsulation of phosphotungstic acid (PTA) within the nanocages of MIL-101 has been achieved via bottle around ship approach under static condition. XRD, FT-IR, P-31 MAS NMR, N-2 adsorption, SEM-EDS and XRF confirm the incorporation and well-distribution of PTA in both middle and large cavities of the MIL-101. SEM, XRD and TEM reveal the dominant crystal shapes of high loading PTA@MIL-101 are a monolithic and the adjacent lattice planes of MIL-101 are larger due to the addition of PTA. The host-guest composite materials PTA@MIL-101 containing 17-50 wt.% of PTA have been obtained and demonstrate an excellent catalytic performance in the oxidative desulfurization process of the refractory sulfur-containing compounds. This is the first example of the application of MIL-101 or PTA@MIL-101 composite materials in oxidative desulfurization. The reactivity of the sulfur-containing compounds follows the order DBT > 4,6-DMDBT > BT. In four consecutive reaction cycles, the catalyst recovery is in excess of 71%, while the DBT conversion slightly decreases. (C) 0 2012 Elsevier Inc. All rights reserved.
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