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Solvent-Free Synthetic Route for Cerium(IV) Metal–Organic Frameworks with UiO-66 Architecture and Their Photocatalytic Applications

Matteo Campanelli, Tiziana Del Giacco, Filippo De Angelis, Edoardo Mosconi, Marco Taddei Orcid Logo, Fabio Marmottini, Roberto D’Amato, Ferdinando Costantino

ACS Applied Materials & Interfaces, Volume: 11, Issue: 48, Pages: 45031 - 45037

Swansea University Author: Marco Taddei Orcid Logo

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DOI (Published version): 10.1021/acsami.9b13730

Abstract

A near solvent-free synthetic route for Ce-UiO-66 metal–organic frameworks (MOFs) is presented. The MOFs are obtained by energetically grinding the reagents, cerium ammonium nitrate (CAN) and the carboxylic linkers, in a mortar for a few minutes with the addition of a small amount of acetic acid (Ac...

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Published in: ACS Applied Materials & Interfaces
ISSN: 1944-8244 1944-8252
Published: American Chemical Society (ACS) 2019
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URI: https://cronfa.swan.ac.uk/Record/cronfa53025
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Abstract: A near solvent-free synthetic route for Ce-UiO-66 metal–organic frameworks (MOFs) is presented. The MOFs are obtained by energetically grinding the reagents, cerium ammonium nitrate (CAN) and the carboxylic linkers, in a mortar for a few minutes with the addition of a small amount of acetic acid (AcOH) as a modulator (8.75 equiv, 0.5 mL). The slurry is then transferred into a 2 mL vial and heated at 120 °C for 1 day. The MOFs have been characterized for their composition, crystallinity, and porosity and employed as heterogeneous catalysts for the photo-oxidation reaction of substituted benzylic alcohols to benzaldaldehydes under near-ultraviolet light irradiation. The catalytic performances, such as selectivity, conversion, and kinetics, exceed those of similar systems studied by chemical oxidation using similar Ce-MOFs as a catalyst. Moreover, the MOFs were found to be reusable up to three cycles without loss of activity. Density functional theory (DFT) calculations were used to fully describe the electronic structure of the best performing MOFs and to provide useful information on the catalytic activity experimentally observed.
Keywords: metal−organic frameworks, cerium, photocatalysis, DFT calculations, green syntheses
College: Professional Services
Issue: 48
Start Page: 45031
End Page: 45037