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Use of a Metallopeptide-Based Mimic Provides Evidence for a Proton-Coupled Electron-Transfer Mechanism for Superoxide Reduction by Nickel-Containing Superoxide Dismutase

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  • This work was supported by the National Science Foundation (CHE-0844234). X-ray absorption measurements were collected on X19a and X3b at the National Synchrotron Light Source (NSLS) which is funded by the DOE (contract no. DE-AC02-98CH10886). Work on X3b, which is part of the Case Center for Synchrotron Bioscience, was also supported by the NIH (P30-EB-009998). Profs. J. Mayer (Univ. of Washington), H. K. Shin (UNR), and an anonymous reviewer are acknowledged for valuable advice.

Abstract

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Für mechanistische Studien der Superoxid-Reduktion durch Nickel-haltige Superoxid-Dismutase wurde ein Metallopeptid-Mimetikum verwendet. Kinetische Untersuchungen deuten auf einen protonengekoppelten Elektronentransfer hin; große kinetische H-D-Isotopeneffekte (KIE) wurden beobachtet. XAS-Analysen zufolge könnte das H-Atom aus einer NiII-S(H)-Cys-Einheit übertragen werden (siehe Diagramm).

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