Supramolecular water oxidation with rubda-based catalysts

Craig J. Richmond, Roc Matheu, Albert Poater, Laura Falivene, Jordi Benet-Buchholz, Xavier Sala, Luigi Cavallo, Antoni Llobet

Research output: Contribution to journalArticleResearchpeer-review

49 Citations (Scopus)

Abstract

© 2014 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. Extremely slow and extremely fast new water oxidation catalysts based on the Rubda (bda = 2,2′-bipyri-dine-6,6′-dicarboxylate) systems are reported with turnover frequencies in the range of 1 and 900 cycless"1, respectively. Detailed analyses of the main factors involved in the water oxidation reaction have been carried out and are based on a combination of reactivity tests, electrochemical experiments, and DFT calculations. These analyses give a convergent interpretation that generates a solid understanding of the main factors involved in the water oxidation reaction, which in turn allows the design of catalysts with very low energy barriers in all the steps involved in the water oxidation catalytic cycle. We show that for this type of system p-stacking interactions are the key factors that influence reactivity and by adequately controlling them we can generate exceptionally fast water oxidation catalysts.
Original languageEnglish
Pages (from-to)17282-17286
JournalChemistry - A European Journal
Volume20
Issue number52
DOIs
Publication statusPublished - 22 Dec 2014

Keywords

  • DFT calculations
  • Redox catalysis
  • Ruthenium
  • Supramolecular chemistry
  • Water splitting

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