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Electrochemically Driven Water Oxidation by a Highly Active Ruthenium-Based Catalyst
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.ORCID-id: 0000-0002-7249-7437
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.ORCID-id: 0000-0001-9329-0091
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Antal upphovsmän: 112019 (Engelska)Ingår i: ChemSusChem, ISSN 1864-5631, E-ISSN 1864-564X, Vol. 12, nr 10, s. 2251-2262Artikel i tidskrift (Refereegranskat) Published
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)].

Ort, förlag, år, upplaga, sidor
2019. Vol. 12, nr 10, s. 2251-2262
Nyckelord [en]
artificial photosynthesis, electrocatalysis, homogeneous catalysis, ruthenium, water oxidation, Green & Sustainable Science & Technology
Nationell ämneskategori
Kemi
Identifikatorer
URN: urn:nbn:se:su:diva-171162DOI: 10.1002/cssc.201900097ISI: 000472806800021PubMedID: 30759324OAI: oai:DiVA.org:su-171162DiVA, id: diva2:1350456
Tillgänglig från: 2019-09-11 Skapad: 2019-09-11 Senast uppdaterad: 2019-12-09Bibliografiskt granskad

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Shatskiy, AndreyOschmann, MichaelMatheu, RocBenet-Buchholz, JordiEriksson, LarsLlobet, AntoniÅkermark, Björn
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Institutionen för organisk kemiInstitutionen för material- och miljökemi (MMK)
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