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A Solvent Free Synthetic Route for Cerium(IV) Metal-Organic Frame-works with UiO-66 Architecture and Their Photocatalytic Application

preprint
revised on 07.10.2019, 14:45 and posted on 07.10.2019, 22:14 by Matteo Campanelli, Tiziana Del Giacco, Filippo De Angelis, Edoardo Mosconi, Marco Taddei, Fabio Marmottini, Ferdinando Costantino

A novel solvent-free synthesis for Ce-UiO-66 metal-organic frameworks (MOFs) is presented. The MOFs are obtained by simply grinding the reagents, cerium ammonium nitrate (CAN) and the carboxylic linkers, in a mortar for few minutes with the addition of a small amount of acetic acid (AcOH) as modulator (1.75 eq, o.1 ml). The slurry is then transferred into a 1 ml vial and heated at 120°C for 1 day. The MOFs have been characterized for their composition, crystallinity and porosity and employed as heterogenous catalysts for the photo-oxidation reaction of substituted benzylic alcohols to benzaldaldehydes under near ultraviolet light irradiation. The catalytic performances, such as yield, conversion and kinetics, exceed those of similar systems studied by chemical oxidation and using Ce-MOF as catalyst. Moreover, the MOFs were found to be reusable up to three cycles without loss of activity. Density functional theory (DFT) calculations gave an estimation of the band-gap shift due to the different nature of the linkers used and provide useful information on the catalytic activity experimentally observed.

Funding

The present work was supported by Fondo Ricerca di Base (FRB-2017) and the Project AMIS, Department of Excellence University of Perugia . M.T. acknowledge the European Un-ion’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No 663830 (M.T.), and the Engineering and Physical Sciences Research Council (EPSRC) for funding through the First Grant scheme EP/R01910X/1.

History

Email Address of Submitting Author

ferdinando.costantino@unipg.it

Institution

University of Perugia

Country

Italy

ORCID For Submitting Author

0000-0002-2120-1456

Declaration of Conflict of Interest

Authors declare no conflict of interest

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