Metal–organic frameworks of the MIL-101 family as heterogeneous single-site catalysts by Nataliya...

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Metal–organic frameworks of the MIL-101 family as heterogeneous single-site catalysts by Nataliya V. Maksimchuk, Olga V. Zalomaeva, Igor Y. Skobelev, Konstantin A. Kovalenko, Vladimir P. Fedin, and Oxana A. Kholdeeva Proceedings A Volume 468(2143):2017-2034 July 8, 2012 ©2012 by The Royal Society

Transcript of Metal–organic frameworks of the MIL-101 family as heterogeneous single-site catalysts by Nataliya...

Page 1: Metal–organic frameworks of the MIL-101 family as heterogeneous single-site catalysts by Nataliya V. Maksimchuk, Olga V. Zalomaeva, Igor Y. Skobelev, Konstantin.

Metal–organic frameworks of the MIL-101 family as heterogeneous single-site catalysts

by Nataliya V. Maksimchuk, Olga V. Zalomaeva, Igor Y. Skobelev, Konstantin A. Kovalenko, Vladimir P. Fedin, and Oxana A. Kholdeeva

Proceedings AVolume 468(2143):2017-2034

July 8, 2012

©2012 by The Royal Society

Page 2: Metal–organic frameworks of the MIL-101 family as heterogeneous single-site catalysts by Nataliya V. Maksimchuk, Olga V. Zalomaeva, Igor Y. Skobelev, Konstantin.

Schematic of MIL-101 structure.

Nataliya V. Maksimchuk et al. Proc. R. Soc. A 2012;468:2017-2034

©2012 by The Royal Society

Page 3: Metal–organic frameworks of the MIL-101 family as heterogeneous single-site catalysts by Nataliya V. Maksimchuk, Olga V. Zalomaeva, Igor Y. Skobelev, Konstantin.

Formation of coordinatively unsaturated chromium sites in the Cr3O-carboxylate cluster of the MIL-101 structure.

Nataliya V. Maksimchuk et al. Proc. R. Soc. A 2012;468:2017-2034

©2012 by The Royal Society

Page 4: Metal–organic frameworks of the MIL-101 family as heterogeneous single-site catalysts by Nataliya V. Maksimchuk, Olga V. Zalomaeva, Igor Y. Skobelev, Konstantin.

Effect of Cr-MIL-101 activation on its catalytic properties in cyclohexene oxidation with TBHP. Reaction conditions: 0.1 M cyclohexene, 0.17 M TBHP, 2.5 mg Cr-MIL-101, 1 ml benzene, 50°C, 10 

h.

Nataliya V. Maksimchuk et al. Proc. R. Soc. A 2012;468:2017-2034

©2012 by The Royal Society

Page 5: Metal–organic frameworks of the MIL-101 family as heterogeneous single-site catalysts by Nataliya V. Maksimchuk, Olga V. Zalomaeva, Igor Y. Skobelev, Konstantin.

(a) Hot catalyst filtration test and (b) catalyst reuse for Cr-MIL-101-catalysed oxidation of cyclohexene with TBHP. Reaction conditions as in figure 3.

Nataliya V. Maksimchuk et al. Proc. R. Soc. A 2012;468:2017-2034

©2012 by The Royal Society

Page 6: Metal–organic frameworks of the MIL-101 family as heterogeneous single-site catalysts by Nataliya V. Maksimchuk, Olga V. Zalomaeva, Igor Y. Skobelev, Konstantin.

XRD patterns for Cr-MIL-101: (a) initial, (b) after treatment with 0.5 M TBHP in MeCN at 80°C for 10 h, and (c) after cyclohexene oxidation with TBHP.

Nataliya V. Maksimchuk et al. Proc. R. Soc. A 2012;468:2017-2034

©2012 by The Royal Society

Page 7: Metal–organic frameworks of the MIL-101 family as heterogeneous single-site catalysts by Nataliya V. Maksimchuk, Olga V. Zalomaeva, Igor Y. Skobelev, Konstantin.

FT-IR spectra of Fe-MIL-101: (a) initial, (b) after four runs of solvent-free cyclohexene oxidation with O2 and (c) after five runs of solvent-free cyclohexane oxidation with TBHP.

Nataliya V. Maksimchuk et al. Proc. R. Soc. A 2012;468:2017-2034

©2012 by The Royal Society

Page 8: Metal–organic frameworks of the MIL-101 family as heterogeneous single-site catalysts by Nataliya V. Maksimchuk, Olga V. Zalomaeva, Igor Y. Skobelev, Konstantin.

Effect of cyclohexane/TBHP molar ratio on the selectivity of cyclohexane oxidation and TBHP efficiency in the presence Cr-MIL-101 (70°C, 8 h).

Nataliya V. Maksimchuk et al. Proc. R. Soc. A 2012;468:2017-2034

©2012 by The Royal Society

Page 9: Metal–organic frameworks of the MIL-101 family as heterogeneous single-site catalysts by Nataliya V. Maksimchuk, Olga V. Zalomaeva, Igor Y. Skobelev, Konstantin.

Hot catalyst filtration test for the coupling reaction of styrene oxide and CO2 over Fe-MIL-101.

Nataliya V. Maksimchuk et al. Proc. R. Soc. A 2012;468:2017-2034

©2012 by The Royal Society