Au@UiO-66: a base free oxidation catalyst

K. Leus; P. Concepcion; M. Vandichel; M. Meledina; A. Grirrane; D. Esquivel; S. Turner; D. Poelman; M. Waroquier; V. Van Speybroeck; G. Van Tendeloo; H. García; P. Van Der Voort

doi:10.1039/C4RA16800C

Au@UiO-66: a base free oxidation catalyst†

K. Leus,^a P. Concepcion,^b M. Vandichel,^c M. Meledina,^d A. Grirrane,^b D. Esquivel,^a S. Turner,^d D. Poelman,^e M. Waroquier,^c V. Van Speybroeck,^c G. Van Tendeloo,^d H. García^b and P. Van Der Voort*^a

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^a Department of Inorganic and Physical Chemistry, Center for Ordered Materials, Organometallics and Catalysis (COMOC), Ghent University, Krijgslaan 281-S3, 9000 Ghent, Belgium
E-mail: pascal.VanDerVoort@ugent.be

^b Instituto de Tecnología Química, CSIC-UPV, Universidad Politécnica de Valencia, Av. de los Naranjos s/n, 46022 Valencia, Spain

^c Center for Molecular Modeling, Ghent University, Technologiepark 903, 9052 Zwijnaarde, Belgium

^d Electron Microscopy for Materials Science (EMAT), University of Antwerp, Groenenborgerlaan 171, 2020 Antwerp, Belgium

^e Department of Solid State Sciences, Lumilab, Ghent University, Krijgslaan 281-S1, 9000 Ghent, Belgium

Abstract

We present the in situ synthesis of Au nanoparticles within the Zr based Metal Organic Framework, UiO-66. The resulting Au@UiO-66 materials were characterized by means of N₂ sorption, XRPD, UV-Vis, XRF, XPS and TEM analysis. The Au nanoparticles (NP) are homogeneously distributed along the UiO-66 host matrix when using NaBH₄ or H₂ as reducing agents. The Au@UiO-66 materials were evaluated as catalysts in the oxidation of benzyl alcohol and benzyl amine employing O₂ as oxidant. The Au@MOF materials exhibit a very high selectivity towards the ketone (up to 100%). Regenerability and stability tests demonstrate that the Au@UiO-66 catalyst can be recycled with a negligible loss of Au species and no loss of crystallinity. In situ IR measurements of UiO-66 and Au@UiO-66-NaBH₄, before and after treatment with alcohol, showed an increase in IR bands that can be assigned to a combination of physisorbed and chemisorbed alcohol species. This was confirmed by velocity power spectra obtained from the molecular dynamics simulations. Active peroxo and oxo species on Au could be visualized with Raman analysis.

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Au@UiO-66: a base free oxidation catalyst†

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