期刊
ACS APPLIED MATERIALS & INTERFACES
卷 11, 期 48, 页码 45031-45037出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.9b13730
关键词
metal-organic frameworks; cerium; photocatalysis; DFT calculations; green syntheses
资金
- Fondo Ricerca di Base (FRB-2017)
- Project AMIS, Department of Excellence University of Perugia
- European Union [663830]
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 degrees 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.
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