Direct-Coupling O₂ Bond Forming Pathway in Cobalt Oxide Water Oxidation Catalysts
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 wi...
| Main Authors: | , |
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| Format: | Article |
| Language: | en_US |
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American Chemical Society
2012
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| Online Access: | http://hdl.handle.net/1721.1/73954 https://orcid.org/0000-0001-7111-0176 |
| _version_ | 1826189392861986816 |
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| author | Wang, Lee-Ping Van Voorhis, Troy |
| author2 | Massachusetts Institute of Technology. Department of Chemistry |
| author_facet | Massachusetts Institute of Technology. Department of Chemistry Wang, Lee-Ping Van Voorhis, Troy |
| author_sort | Wang, Lee-Ping |
| collection | MIT |
| description | 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. |
| first_indexed | 2024-09-23T08:13:59Z |
| format | Article |
| id | mit-1721.1/73954 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T08:13:59Z |
| publishDate | 2012 |
| publisher | American Chemical Society |
| record_format | dspace |
| spelling | mit-1721.1/739542022-09-30T08:29:04Z Direct-Coupling O₂ Bond Forming Pathway in Cobalt Oxide Water Oxidation Catalysts Wang, Lee-Ping Van Voorhis, Troy Massachusetts Institute of Technology. Department of Chemistry Van Voorhis, Troy Wang, Lee-Ping Van Voorhis, Troy 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. eni-MIT Solar Frontiers Center (Solar Frontiers Research Program) 2012-10-15T14:16:45Z 2012-10-15T14:16:45Z 2011-08 2011-07 Article http://purl.org/eprint/type/JournalArticle 1948-7185 http://hdl.handle.net/1721.1/73954 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. https://orcid.org/0000-0001-7111-0176 en_US http://dx.doi.org/ 10.1021/jz201021n Journal of Physical Chemistry Letters Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. application/pdf American Chemical Society Prof. van Voorhis via Erja Kajosalo |
| spellingShingle | Wang, Lee-Ping Van Voorhis, Troy Direct-Coupling O₂ Bond Forming Pathway in Cobalt Oxide Water Oxidation Catalysts |
| title | Direct-Coupling O₂ Bond Forming Pathway in Cobalt Oxide Water Oxidation Catalysts |
| title_full | Direct-Coupling O₂ Bond Forming Pathway in Cobalt Oxide Water Oxidation Catalysts |
| title_fullStr | Direct-Coupling O₂ Bond Forming Pathway in Cobalt Oxide Water Oxidation Catalysts |
| title_full_unstemmed | Direct-Coupling O₂ Bond Forming Pathway in Cobalt Oxide Water Oxidation Catalysts |
| title_short | Direct-Coupling O₂ Bond Forming Pathway in Cobalt Oxide Water Oxidation Catalysts |
| title_sort | direct coupling o₂ bond forming pathway in cobalt oxide water oxidation catalysts |
| url | http://hdl.handle.net/1721.1/73954 https://orcid.org/0000-0001-7111-0176 |
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