Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 140, Issue 29, Pages 9042-9045Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b04671
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Funding
- NIH [DK031450, GM28962]
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[(L)Cu-II(O-2(center dot-)](+) (i.e., cupric-superoxo) complexes, as the first and/or key reactive intermediates in (bio)chemical Cu-oxidative processes, including in the monooxygenases PHM and D beta M, have been systematically stabilized by intramolecular hydrogen bonding within a TMPA ligand-based framework. Also, gradual strengthening of ligand-derived H-bonding dramatically enhances the [(L)Cu-II(O-2(center dot-)](+) reactivity toward hydrogen-atom abstraction (HAA) of phenolic O-H bonds. Spectroscopic properties of the superoxo complexes and their azido analogues, [(L)Cu-II(N-3(-)](+), also systematically change as a function of ligand H-bonding capability.
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