Change search
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • harvard1
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf
Electrochemically Driven Water Oxidation by a Highly Active Ruthenium-Based Catalyst
Stockholm Univ, Arrhenius Lab, Dept Organ Chem, Svante Arrhenius Vag 16C, S-10691 Stockholm, Sweden..ORCID iD: 0000-0002-7249-7437
Stockholm Univ, Arrhenius Lab, Dept Organ Chem, Svante Arrhenius Vag 16C, S-10691 Stockholm, Sweden.;Russian Acad Sci, Inst Problems Chem Phys, Academician Semenovs Prospect 1g, Moscow 142432, Russia..
Stockholm Univ, Arrhenius Lab, Dept Organ Chem, Svante Arrhenius Vag 16C, S-10691 Stockholm, Sweden..
BIST, Inst Chem Res Catalonia ICIQ, Avinguda Paisos Catalans 16, Tarragona 43007, Spain..ORCID iD: 0000-0001-8601-5219
Show others and affiliations
2019 (English)In: ChemSusChem, ISSN 1864-5631, E-ISSN 1864-564X, Vol. 12, no 10, p. 2251-2262Article in journal (Refereed) 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)].

Place, publisher, year, edition, pages
Wiley-VCH Verlagsgesellschaft, 2019. Vol. 12, no 10, p. 2251-2262
Keywords [en]
artificial photosynthesis, electrocatalysis, homogeneous catalysis, ruthenium, water oxidation
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:kth:diva-255333DOI: 10.1002/cssc.201900097ISI: 000472806800021PubMedID: 30759324Scopus ID: 2-s2.0-85064528579OAI: oai:DiVA.org:kth-255333DiVA, id: diva2:1340810
Note

QC 20190806

Available from: 2019-08-06 Created: 2019-08-06 Last updated: 2019-08-06Bibliographically approved

Open Access in DiVA

No full text in DiVA

Other links

Publisher's full textPubMedScopus

Authority records BETA

Kärkäs, Markus D.

Search in DiVA

By author/editor
Shatskiy, AndreyMatheu, RocBenet-Buchholz, JordiKärkäs, Markus D.Llobet, Antoni
By organisation
Organic chemistry
In the same journal
ChemSusChem
Chemical Sciences

Search outside of DiVA

GoogleGoogle Scholar

doi
pubmed
urn-nbn

Altmetric score

doi
pubmed
urn-nbn
Total: 20 hits
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • harvard1
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf