Clerick, Sander

De Canck, Els

Hong, Mei

Van Der Voort, Pascal

English

Ghent University Academic Bibliography

Molybdenum(VI) Dioxo Complexes Supported on stable Ring-type Periodic Mesoporous Organosilicas Mei Hong, Sander Clerick, Els De Canck, Pascal Van Der Voort* Department of Inorganic and Physical Chemistry, Center for Ordered Materials, Organometallics and Catalysis (COMOC), Ghent University, Krijgslaan 281-S3, 9000 Ghent, Belgium.  In the past decades, high-valence oxomolybdenum complexes have proven to be excellent catalysts for the reduction and oxidation of organic compounds [1-3] but can also act as a Lewis acid [4]. We report the synthesis of a heterogeneous molybdenum dioxo-catalyst with high selective catalytic performance, by grafting a molecular molybdenum dioxo-precursor onto a Periodic Mesoporous Organosilica (PMO) (Scheme). A 100% monoallyl ring-type PMO [5] was functionalized with acetylacetone via a radical reaction. A molybdenum dioxo complex, using the solvent adduct [MoO2Cl2(THF)2] was then immobilized on the allyl bearing  PMO material in order to prepare a new molybdenum (VI) based heterogenous catalyst. Structural analyses by X-ray powder diffraction, nitrogen sorption and transmission electron microscopy showed an ordered mesostructure while characterization by infrared and X-ray photoelectron spectroscopy demonstrated molybdenum (VI) active centers supported on the PMO material. The catalytic activity of the supported catalyst was tested in the aerobic oxidation of 5-hydroxymethylfurfural (HMF).                                                                                                                                                    mAR                 mAR-acac                                    MoO2Cl2@mAR-acac   Scheme Schematic representation of the anchoring of MoO2Cl2(THF)2 onto the monoallyl ring PMO.                                                                                             [1] Korstanje, T.J. Kleijn, H. Jastrzebski J.T.B.H. and Klein Gebbink R.J.M. Green Chem. 15 (2013) 982. [2] Fernandes T.A. and Fernandes A.C., ChemCatChem. 7 (2015) 3503. [3] García, N. Rubio-Presa, R. García-García, P. Fernández-Rodríguez, M.A. Pedrosa, M.R. Arnáiza F.J. and Sanz. R., Green Chem.18 (2016) 2335. [4] Guggilapu, S.D. Prajapti, S.K. Nagarsenkar, A. Lalita G., Vegi G.M.N. and Babu B. N., New J. Chem. 40 (2016) 838. [5] Clerick, S. De Canck, E. Hendrickx, K. Van Speybroeck V. and Van Der Voort P., Green Chem. 18 (2016) 6035.  E-mail: Pascal.VanDerVoort@UGent.be;  www: http://www.comoc.ugent.be. sisisiOOO OHO OOOMoOOClMn(OAc)3       AcOHsiisiisiiOOO OHO OOOMoO2Cl2(THF)2THF

Molybdenum(VI) dioxo complexes supported on stable ring-type periodic mesoporous organosilicas

https://biblio.ugent.be/publication/8517330/file/8517332.pdf

Molybdenum(VI) dioxo complexes supported on stable ring-type periodic mesoporous organosilicas

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Ghent University Academic Bibliography