Carbon‐Nanotube‐Appended PAMAM Dendrimers Bearing Iron(II) α‐Keto Acid Complexes: Catalytic Non‐Heme Oxygenase Models
(2019) Chemistry: A European Journal — Vol. 25, p. 9191-9196 (2019)
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- Authors
Sheet, Debobrata 
- Abstract
- Poly(amidoamine) dendrimers grafted on carbon nanotubes have been appended with iron(II)-α-Keto acid (benzoylformate) complex of polypyridyl ligand to design artificial nonheme oxygenase model. This nano-enzyme was applied for selective catalytic oxidation of organic molecules. While the carbon nanotubes serve as robust heterogeneous platform, the amineterminals of dendrimers provide catalysts binding sites and the amidebonds provide a necessary second coordination sphere similar to the enzymatic polypeptide chains. Such hybrid design prevented wrecking down of the primary active sites leading to 8 times faster oxidative decarboxylation rates than its homogeneous analogue. An electrophilic iron(IV)-oxo intermediate has been intercepted that catalyzes the selective oxidation of alcohols to aldehydes and incorporates single oxygen atoms into sulfides and olefins 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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Citations
Sheet, D., Bera, A., Fu, Y., Desmecht, A., Riant, O., & Hermans, S. (2019). Carbon‐Nanotube‐Appended PAMAM Dendrimers Bearing Iron(II) α‐Keto Acid Complexes: Catalytic Non‐Heme Oxygenase Models. Chemistry: A European Journal, 25, 9191-9196. https://doi.org/10.1002/chem.201901735 (Original work published 2019)