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Synthesis and characterization of open and sandwich-type polyoxometalates reveals visible-light-driven water oxidation via POM-photosensitizer complexes


Car, Pierre-Emmanuel; Guttentag, Miguel; Baldridge, Kim K; Alberto, Roger; Patzke, Greta R (2012). Synthesis and characterization of open and sandwich-type polyoxometalates reveals visible-light-driven water oxidation via POM-photosensitizer complexes. Green Chemistry, 14(6):1680-1688.

Abstract

The trivacant triruthenium-substituted polyoxometalate α-K6Na[{Ru3O3(H2O)Cl2}(SiW9O34)]·17H2O (1) and two sandwich-type Co- and Ni-containing silicotungstates K11Na1[M4(H2O)2(SiW9O34)2]·nH2O (M = Co2+, Ni2+) (2, 3) based on the same Keggin-type building block were obtained through variation of a solution-based protocol. All compounds were investigated with respect to their performance as visible-light-driven water oxidation catalysts (WOCs). Analytical characterizations and photocatalytic reactivity of (1) are correlated with results of B97D/Def2-TZVP computation. The WOC activity of (1) and (2) was found to arise from their immobilization into a recyclable POM–photosensitizer complex (POM–PS). These POM–PS complexes are formed in the initial phase of the reaction, and they prevent POM decomposition into colloidal oxide catalysts.

The trivacant triruthenium-substituted polyoxometalate α-K6Na[{Ru3O3(H2O)Cl2}(SiW9O34)]·17H2O (1) and two sandwich-type Co- and Ni-containing silicotungstates K11Na1[M4(H2O)2(SiW9O34)2]·nH2O (M = Co2+, Ni2+) (2, 3) based on the same Keggin-type building block were obtained through variation of a solution-based protocol. All compounds were investigated with respect to their performance as visible-light-driven water oxidation catalysts (WOCs). Analytical characterizations and photocatalytic reactivity of (1) are correlated with results of B97D/Def2-TZVP computation. The WOC activity of (1) and (2) was found to arise from their immobilization into a recyclable POM–photosensitizer complex (POM–PS). These POM–PS complexes are formed in the initial phase of the reaction, and they prevent POM decomposition into colloidal oxide catalysts.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Language:English
Date:5 April 2012
Deposited On:24 Jan 2013 15:53
Last Modified:05 Apr 2016 16:20
Publisher:
Publisher DOI:https://doi.org/10.1039/c2gc16646a

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