Synthesis and characterisation of novel ruthenium multi-substituted polyoxometalates: alpha,beta-[SiW9O37Ru4(H2O)(3)Cl-3](7-)
authors Gamelas, JAF; Carapuca, HM; Balula, MS; Evtuguin, DV; Schlindwein, W; Figueiras, FG; Amaral, VS; Cavaleiro, AMV
nationality International
journal POLYHEDRON
author keywords Ruthenium; Polyoxometalate; Transition metal-substituted; polyoxotungstate; Trilacunary; Keggin
keywords KEGGIN-TYPE POLYOXOTUNGSTATES; SUBSTITUTED POLYOXOMETALATE; STRUCTURAL-CHARACTERIZATION; ELECTROCHEMICAL-BEHAVIOR; HYDROTHERMAL SYNTHESIS; CATALYTIC CHEMISTRY; MAGNETIC-PROPERTIES; ALKENE OXIDATION; MOLECULAR-OXYGEN; WATER OXIDATION
abstract Novel ruthenium multi-substituted polyoxometalate compounds of general formulae K6Na[SiW9O37Ru4III(H2O)(3)Cl-3]center dot nH(2)O (alpha- and beta-SiW9O34 isomers) were synthesised via the reactions of the trilacunary Keggin alpha- and beta-[SiW9O34](10-) anions with RuCl3 in aqueous solution. Characterisation was performed by analytical, spectroscopic, magnetic, and electrochemical techniques. The results are in accordance with the new polyoxometalates having the trivacant Keggin anion (alpha or beta isomer) linked to a cubane-type Ru4O4 cluster. The co-ordination sphere of ruthenium is completed with water molecules and chloride anions. Magnetic measurements showed that the majority of the molecules have the Ru ions cluster in a compensated configuration constrained to an antiferromagnetic alignment at very low temperature and following a Curie-Weiss like behaviour. For both isomers, cyclic voltammetry revealed quasi-reversible redox processes at the ruthenium centres, namely Ru-IV/III and Ru-III/II, which were found to be pH dependent. The novel polyoxotungstates incorporate the highest content of ruthenium (W:Ru = 2.25:1) ever reported for Keggin-, Dawson or sandwich-type transition metal-substituted polyoxometalates and may find promising applications as oxidative catalysts. (C) 2010 Elsevier Ltd. All rights reserved.
publisher PERGAMON-ELSEVIER SCIENCE LTD
issn 0277-5387
year published 2010
volume 29
issue 16
beginning page 3066
ending page 3073
digital object identifier (doi) 10.1016/j.poly.2010.08.002
web of science category Chemistry, Inorganic & Nuclear; Crystallography
subject category Chemistry; Crystallography
unique article identifier WOS:000284392100007
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  impact metrics
times cited (wos core): 13
journal impact factor (jcr 2016): 1.926
5 year journal impact factor (jcr 2016): 1.790
category normalized journal impact factor percentile (jcr 2016): 52.592
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