| Water Exchange Reactivity and Stability of Cobalt Polyoxometalates under Catalytically Relevant pH Conditions: Insight into Water Oxidation Catalysis. | |
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MedLine Citation:
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PMID: 21809868 Owner: NLM Status: Publisher |
Abstract/OtherAbstract:
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Water exchange on a molecular, purely inorganic cobalt-based water oxidation catalyst, [Co(4)(II)(H(2)O)(2)(α-P(1)W(9)O(34))(2)](10-) (1), in the catalytically relevant pH region (pH 6-10) is studied using (17)O-NMR spectroscopy and ultrahigh-resolution electrospray ionization mass spectrometry. The results are compared with those of the inactive [Co(II)(H(2)O)(1)Si(1)W(11)O(39)](6-) (2), which is stable in the same pH region. The results obtained provide mechanistic details of the elementary reaction step related to the water oxidation on homogeneous metal oxide catalysts under catalytically relevant conditions. It is shown that the structural integrity of 1 and 2 is maintained, no deprotonation of the aqua ligands on the Co(II) centers occurs, and the water exchange does not undergo any mechanistic changeover at the catalytic pH conditions. We have demonstrated that the water exchange process is influenced by the cluster environment surrounding the water binding sites and is fast enough to not be rate-limiting for the water oxidation catalysis. |
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Authors:
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Dominik Lieb; Achim Zahl; Elizabeth F Wilson; Carsten Streb; Leanne C Nye; Karsten Meyer; Ivana Ivanović-Burmazović |
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Publication Detail:
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Type: JOURNAL ARTICLE Date: 2011-8-2 |
Journal Detail:
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Title: Inorganic chemistry Volume: - ISSN: 1520-510X ISO Abbreviation: - Publication Date: 2011 Aug |
Date Detail:
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Created Date: 2011-8-3 Completed Date: - Revised Date: - |
Medline Journal Info:
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Nlm Unique ID: 0366543 Medline TA: Inorg Chem Country: - |
Other Details:
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Languages: ENG Pagination: - Citation Subset: - |
Affiliation:
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Department of Chemistry and Pharmacy, University of Erlangen-Nürnberg , Egerlandstr. 1, 91058 Erlangen, Germany. |
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From MEDLINE®/PubMed®, a database of the U.S. National Library of Medicine
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