Supramolecular water oxidation with rubda-based catalysts

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

Research output: Contribution to journalArticlepeer-review

67 Scopus citations

Abstract

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 (US)
Pages (from-to)17282-17286
Number of pages5
JournalChemistry - A European Journal
Volume20
Issue number52
DOIs
StatePublished - Nov 5 2014

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: C.R. thanks the European Commission and the Marie Curie Actions for an Intra-European Fellowship. A.L. thanks MINECO CTQ-2013-49075-R and "La Caixa" foundation for financial support. R.M. thanks "La Caixa" foundation for a Ph.D. grant. X.S. thanks MINECO CTQ2011-26440 for financial support. L.C. thanks King Abdullah University of Science and Technology for financial support. A.P. thanks the Spanish MINECO for a Ramon y Cajal contract (RYC-2009-05226) and European Commission for a Career Integration Grant (CIG09-GA-2011-293900).

ASJC Scopus subject areas

  • Chemistry(all)

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