AuthorsRichmond, Craig J.
Llobet, Antoni A.
KAUST DepartmentBiological and Environmental Sciences and Engineering (BESE) Division
Chemical Science Program
KAUST Catalysis Center (KCC)
Physical Science and Engineering (PSE) Division
Online Publication Date2014-11-05
Print Publication Date2014-12-22
Embargo End Date2015-11-05
Permanent link to this recordhttp://hdl.handle.net/10754/563846
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AbstractExtremely 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.
SponsorsC.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).
JournalChemistry - A European Journal
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Richmond, C. J., Matheu, R., Poater, A., Falivene, L., Benet-Buchholz, J., Sala, X., … Llobet, A. (2014). CCDC 1014178: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/cc131bfx. DOI: 10.5517/cc131bfx HANDLE: 10754/624353