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Water oxidation by manganese oxides formed from tetranuclear precursor complexes: the influence of phosphate on structure and activity
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC, Analytical Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
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2014 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 16, no 24, 11965-11975 p.Article in journal (Refereed) Published
Abstract [en]

Two types of manganese oxides have been prepared by hydrolysis of tetranuclear Mn(III) complexes in the presence or absence of phosphate ions. The oxides have been characterized structurally using X-ray absorption spectroscopy and functionally by O-2 evolution measurements. The structures of the oxides prepared in the absence of phosphate are dominated by di-mu-oxo bridged manganese ions that form layers with limited long-range order, consisting of edge-sharing MnO6 octahedra. The average manganese oxidation state is +3.5. The structure of these oxides is closely related to other manganese oxides reported as water oxidation catalysts. They show high oxygen evolution activity in a light-driven system containing [Ru(bpy)(3)](2+) and S2O82- at pH 7. In contrast, the oxides formed by hydrolysis in the presence of phosphate ions contain almost no di-mu-oxo bridged manganese ions. Instead the phosphate groups are acting as bridges between the manganese ions. The average oxidation state of manganese ions is +3. This type of oxide has much lower water oxidation activity in the light-driven system. Correlations between different structural motifs and the function as a water oxidation catalyst are discussed and the lower activity in the phosphate containing oxide is linked to the absence of protonable di-mu-oxo bridges.

Place, publisher, year, edition, pages
2014. Vol. 16, no 24, 11965-11975 p.
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Physical Chemistry
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URN: urn:nbn:se:uu:diva-228523DOI: 10.1039/c3cp55125cISI: 000337122000016OAI: oai:DiVA.org:uu-228523DiVA: diva2:734306
Available from: 2014-07-16 Created: 2014-07-16 Last updated: 2017-12-05Bibliographically approved

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Shevchenko, DenysStyring, StenbjornThapper, Anders

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