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  • 1.
    Shatskiy, Andrey
    et al.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Bardin, Andrey A.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Oschmann, Michael
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Matheu, Roc
    Benet-Buchholz, Jordi
    Eriksson, Lars
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Kärkäs, Markus D.
    Johnston, Eric
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Gimbert-Suriñach, Carolina
    Llobet, Antoni
    Åkermark, Björn
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Electrochemically Driven Water Oxidation by a Highly Active Ruthenium-Based Catalyst2019In: ChemSusChem, ISSN 1864-5631, E-ISSN 1864-564X, Vol. 12, no 10, p. 2251-2262Article in journal (Refereed)
    Abstract [en]

    The highly active ruthenium-based water oxidation catalyst [Ru-X(mcbp)(OHn)(py)(2)] [mcbp(2-)=2,6-bis(1-methyl-4-(carboxylate)benzimidazol-2-yl)pyridine; n=2, 1, and 0 for X=II, III, and IV, respectively], can be generated in a mixture of Ru-III and Ru-IV states from either [Ru-II(mcbp)(py)(2)] or [Ru-III(Hmcbp)(py)(2)](2+) precursors. The precursor complexes are isolated and characterized by single-crystal X-ray analysis, NMR, UV/Vis, EPR, and FTIR spectroscopy, ESI-HRMS, and elemental analysis, and their redox properties are studied in detail by electrochemical and spectroscopic methods. Unlike the parent catalyst [Ru(tda) (py)(2)] (tda(2-)=[2,2:6,2-terpyridine]-6,6-dicarboxylate), for which full transformation into the catalytically active species [Ru-IV(tda)(O)(py)(2)] could not be carried out, stoichiometric generation of the catalytically active Ru-aqua complex [Ru-X(mcbp)(OHn)(py)(2)] from the Ru-II precursor was achieved under mild conditions (pH7.0) and short reaction times. The redox properties of the catalyst were studied and its activity for electrocatalytic water oxidation was evaluated, reaching a maximum turnover frequency (TOFmax) of around 40000s(-1) at pH9.0 (from foot-of-the-wave analysis), which is comparable to the activity of the state-of-the-art catalyst [Ru-IV(tda)(O)(py)(2)].

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