Peroxo-Cerium(IV)-Containing Polyoxometalates: Ce(O)(GeWO), a Recyclable Homogeneous Oxidation Catalyst.

08:00 EDT 14th August 2019 | BioPortfolio

Summary of "Peroxo-Cerium(IV)-Containing Polyoxometalates: Ce(O)(GeWO), a Recyclable Homogeneous Oxidation Catalyst."

The class of peroxo-cerium-containing polyoxometalates has been discovered via the synthesis of the 9-peroxo-6-cerium(IV)-containing 30-tungsto-3-germanate, [Ce(O)(GeWO)] (). Polyanion consists of a cyclic [Ce(O)] assembly that is stabilized by three dilacunary [GeWO] Keggin fragments. The title polyanion is solution-stable, on the basis of W nuclear magnetic resonance, and was shown to act as a recyclable homogeneous catalyst for the selective, microwave-activated sulfoxidation of the model substrate methionine to the sulfoxide in the absence and to the sulfone in the presence of hydrogen peroxide. Solution and solid-state Raman as well as solid-state infrared studies of demonstrated the complete loss (and regain) of the nine peroxo groups during the catalytic cycle, suggesting that the peroxo-free {Ce(GeW)} skeleton remains most likely intact during the catalytic cycle. Solid-state X-ray photoelectron spectroscopy measurements showed that peroxo loss is accompanied by reduction of the cerium ions from +4 to +3, which is fully reversible. Density functional theory calculations are in complete agreement with all of these observations and furthermore suggest that the reduction of the six cerium(IV) ions is accompanied by the formation of molecular dioxygen.


Journal Details

This article was published in the following journal.

Name: Inorganic chemistry
ISSN: 1520-510X


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