Cysteinate-ligated heme and non-heme Fe-enzymes play key roles in biological processes that have a tremendous impact on human health, including tumor suppression, and the prevention of neurological disorders such as Parkinson’s, and Alzheimer’s. In some cases (e.g., nitrile hydratases and cysteine dioxygenases) sulfur oxygenation is intimately tied to function. Evidence for mechanistic proposals is, in many cases, lacking, because intermediates have yet to be observed. Using small molecules, we have been able to trap metastable thiolate-ligated Fe-intermediates (oxo atom donor adducts, high-valent oxos, peroxos, and hydroperoxos) and obtain kinetic evidence for key steps in the mechanisms of these enzymes.

Spectroscopic, and/or crystallographic characterization of metastable intermediates involved in cysteinate-ligated non-heme iron-promoted reaction mechanisms

253rd National Meeting (2017)

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