A Dinuclear Ruthenium-Based Water Oxidation Catalyst: Use of Non-Innocent Ligand Frameworks for Promoting Multi-Electron Reactions
2015 (English)In: Chemistry - A European Journal, ISSN 0947-6539, E-ISSN 1521-3765, Vol. 21, no 28, 10039-10048 p.Article in journal (Refereed) Published
Insight into how H2O is oxidized to O-2 is envisioned to facilitate the rational design of artificial water oxidation catalysts, which is a vital component in solar-to-fuel conversion schemes. Herein, we report on the mechanistic features associated with a dinuclear Ru-based water oxidation catalyst. The catalytic action of the designed Ru complex was studied by the combined use of high-resolution mass spectrometry, electrochemistry, and quantum chemical calculations. Based on the obtained results, it is suggested that the designed ligand scaffold in Ru complex 1 has a non-innocent behavior, in which metal-ligand cooperation is an important part during the four-electron oxidation of H2O. This feature is vital for the observed catalytic efficiency and highlights that the preparation of catalysts housing non-innocent molecular frameworks could be a general strategy for accessing efficient catalysts for activation of H2O.
Place, publisher, year, edition, pages
2015. Vol. 21, no 28, 10039-10048 p.
density functional calculations, electrochemistry, ligands, ruthenium, water splitting
Research subject Organic Chemistry
IdentifiersURN: urn:nbn:se:su:diva-119297DOI: 10.1002/chem.201406613ISI: 000357026700014OAI: oai:DiVA.org:su-119297DiVA: diva2:844208