Efficient light-driven water oxidation catalysis by dinuclear ruthenium complexes

Serena Berardi, Laia Francàs, Sven Neudeck, Somnath Maji, Jordi Benet-Buchholz, Franc Meyer, Antoni Llobet

Research output: Contribution to journalArticleResearchpeer-review

25 Citations (Scopus)

Abstract

© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. Mastering the light-induced four-electron oxidation of water to molecular oxygen is a key step towards the achievement of overall water splitting to produce alternative solar fuels. In this work, we report two rugged molecular pyrazolate-based diruthenium complexes that efficiently catalyze visible-light-driven water oxidation. These complexes were fully characterized both in the solid state (by X-ray diffraction analysis) and in solution (spectroscopically and electrochemically). Benchmark performances for homogeneous oxygen production have been obtained for both catalysts in the presence of a photosensitizer and a sacrificial electron acceptor at pH 7, and a turnover frequency of up to 11.1 s-1 and a turnover number of 5300 were obtained after three successive catalytic runs. Under the same experimental conditions with the same setup, the pyrazolate-based diruthenium complexes outperform other well-known water oxidation catalysts owing to both electrochemical and mechanistic aspects. Limelight on water oxidation: Two rugged pyrazolate-based diruthenium complexes efficiently catalyze the homogeneous photoinduced water oxidation in a three-component system including a photosensitizer and a sacrificial electron acceptor at pH 7. Outstanding results are obtained in terms of both turnover number (TON) and turnover frequency (TOF).
Original languageEnglish
Pages (from-to)3688-3696
JournalChemSusChem
Volume8
Issue number21
DOIs
Publication statusPublished - 1 Nov 2015

Keywords

  • complexes
  • photosensitizer
  • redox chemistry
  • ruthenium
  • water oxidation

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