Selective Oxidation of C-H Bonds through a Manganese(III) Hydroperoxo in Mn-Exchanged CFA-1.

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ID: 58120
2019
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Abstract
Partial substitution of Zn by Mn in Zn(OAc)(5,5'-bibenzo[][1,2,3]triazole) (CFA-1) results in a Mn species supported by three nitrogen ligands and a charge-balancing anion, a structure reminiscent of those found in molecular "scorpionate" complexes. Unlike molecular manganese(II) scorpionates, Mn-CFA-1 is capable of catalytically activating oxygen from air to oxidize C-H bonds up to 87 kcal/mol in strength. A series of in situ spectroscopic studies, including diffuse-reflectance UV-vis, diffuse-reflectance infrared Fourier transform spectroscopy, and X-ray absorption spectroscopy, reveal that catalysis likely proceeds through a manganese(III) hydroperoxo that is only accessed in the presence of a hydrogen-atom donor. These results demonstrate that the site isolation provided in metal-organic frameworks enables the generation and utilization of highly reactive species for catalysis that are inaccessible in molecular systems.
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stubbs2019selectiveinorganic Use this key to autocite in the manuscript while using SciMatic Manuscript Manager or Thesis Manager
Authors Stubbs, Amanda W;Dincǎ, Mircea;
Journal Inorganic chemistry
Year 2019
DOI
10.1021/acs.inorgchem.9b02068
URL
Keywords
antioxidant 1,2,3-Triazole antitumor vitamin c hif-1 quantum-chemical modelling

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