Direct-Coupling O₂ Bond Forming Pathway in Cobalt Oxide Water Oxidation Catalysts
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Wang_VV.Cobalt_Catalyst.JPCL.2011.pdf
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Author(s) •
Wang, Lee-Ping
Van Voorhis, Troy
Date Issued
August 2011
Journal
Journal of Physical Chemistry Letters
Publisher
American Chemical Society
Citation
Wang, Lee-Ping, and Troy Van Voorhis. “Direct-Coupling O₂ Bond Forming a Pathway in Cobalt Oxide Water Oxidation Catalysts.” The Journal of Physical Chemistry Letters 2.17 (2011): 2200–2204. Web.
Version
Author's final manuscript
Abstract
We report a catalytic mechanism for water oxidation in a cobalt oxide cubane model compound, in which the crucial O–O bond formation step takes place by direct coupling between two CoIV(O) metal oxo groups. Our results are based upon density functional theory (DFT) calculations and are consistent with experimental studies of the CoPi water oxidation catalyst. The computation of energetics and barriers for the steps leading up to and including the O–O bond formation uses an explicit solvent model within a hybrid quantum mechanics/molecular mechanics (QM/MM) framework, and captures the essential hydrogen-bonding effects and dynamical flexibility of this system.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
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DOI of Published Version
https://doi.org/10.1021/jz201021n