Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 25, Issue 39, Pages 9191-9196Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201901735
Keywords
carbon nanotubes; catalysis; non-heme; oxygen activation; PAMAM dendrimers
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Funding
- Fonds De La Recherche Scientifique - FNRS [FNRS J.0053.17] Funding Source: Medline
- Belspo - Politique Scientifique Federale (Belgique) [Postdoctoral Fellowship] Funding Source: Medline
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Poly(amidoamine) dendrimers grafted on carbon nanotubes have been appended with iron(II)-alpha-keto acid (benzoylformate) complex of polypyridyl ligand to design artificial non-heme oxygenase model. This nano-enzyme was applied for selective catalytic oxidation of organic molecules. Although the carbon nanotubes serve as a robust heterogeneous platform, the amine terminals of dendrimers provide catalysts binding sites and the amide bonds provide a necessary second coordination sphere similar to the enzymatic polypeptide chains. Such a hybrid design prevented the deactivation of the primary active sites leading to 8 times faster oxidative decarboxylation rates than those of its homogeneous analogue. An electrophilic iron(IV)-oxo intermediate has been intercepted, which catalyzes the selective oxidation of alcohols to aldehydes and incorporates single oxygen atoms into sulfides and olefins by using aerial oxygen with multiple turnover numbers. The catalyst was consecutively regenerated three times by mild chemical treatment and showed negligible loss of activity.
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