Biswas, Shyam Prosad

Van Der Voort, Pascal

English

Ghent University Academic Bibliography

Comparing the Sorption and Catalytic Performances of Porous Isostructural V-MIL-47-X (X = -CH3, -Cl, -Br, -OH) Metal-Organic Frameworks   Shyam Biswas and Pascal Van Der Voort; Department of Inorganic and Physical Chemistry, COMOC: Center for Ordered Materials, Organometallics and Catalysis Ghent University  Metal-organic frameworks have attracted a great deal of interest due to their applications in gas storage/separation and catalysis. However, catalytic investigations using MOFs as catalysts are still in their infancy and the catalytic reaction mechanisms in MOFs are still poorly understood.[1] Recently, we have demonstrated[2] the remarkable catalytic performance of the coordinatively saturated V-based MIL-47 in cyclohexene epoxidation using TBHP/decane as the oxidant. In order to verify the effect of functionalization on the catalytic properties of parent MIL-47, we have now introduced four different functionalities (X = -CH3, -Cl, -Br and -OH) into the terephthalate linker. The compounds have been synthesized in a rapid (30 min) microwave irradiation route under hydrothermal conditions (150-170 °C). Thermogravimetric analyses show high thermal stability (250-300 °C). The as-synthesized solids were calcined under dynamic vacuum for overnight to remove the free linkers from the pores and achieve significant microporosity (type-I isotherms, Fig. 1a; SBET: 305-657 m2 g-1). The catalysts have been further characterized by DRIFT, elemental analysis and X-ray powder diffractometry. Employing TBHP/decane as the oxidant, catalytic tests exhibit moderate yields (35-39%, Fig. 1b) of the cyclohexene epoxide for all the catalysts with good regenerability.    Fig. 1. (a) N2 sorption analysis, and (b) time conversion plot of cyclohexene oxide for MIL-47-CH3.  [1] Corma, A., Garcia, H. and Llabres i Xamena, F. H., Chem. Rev. B. 110 (2010) 4606.  [2] Leus, K., Vandichel , M., Liu, Y.-Y., Muylaert, I., Musschoot, J., Pyl, S., Vrielinck, H., Callens, F., Marin, G. B., Detavernier, C., Wiper, P. V., Khimyak, Y. Z., Waroquier, M., Van Speybroeck, V. and Van Der Voort, P., J. Catal. (2011), doi:10.1016/j.jcat.2011.09.014. 

Comparing the sorption and catalytic performances of porous isostructural V-MIL-47-X (X = -CH3, -Cl, -Br, -OH) metal-organic frameworks

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Comparing the sorption and catalytic performances of porous isostructural V-MIL-47-X (X = -CH3, -Cl, -Br, -OH) metal-organic frameworks

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Ghent University Academic Bibliography