Supramolecular water oxidation with rubda-based catalysts

Handle URI:
http://hdl.handle.net/10754/563846
Title:
Supramolecular water oxidation with rubda-based catalysts
Authors:
Richmond, Craig J.; Matheu, Roc; Poater, Albert; Falivene, Laura ( 0000-0003-1509-6191 ) ; Benet-Buchholz, Jordi; Sala, Xavier; Cavallo, Luigi ( 0000-0002-1398-338X ) ; Llobet, Antoni A.
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.
KAUST Department:
Biological and Environmental Sciences and Engineering (BESE) Division; KAUST Catalysis Center (KCC); Physical Sciences and Engineering (PSE) Division; Chemical Science Program
Publisher:
Wiley-Blackwell
Journal:
Chemistry - A European Journal
Issue Date:
5-Nov-2014
DOI:
10.1002/chem.201405144
Type:
Article
ISSN:
09476539
Sponsors:
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).
Is Supplemented By:
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:http://hdl.handle.net/10754/624353
Appears in Collections:
Articles; Physical Sciences and Engineering (PSE) Division; Chemical Science Program; KAUST Catalysis Center (KCC); Biological and Environmental Sciences and Engineering (BESE) Division

Full metadata record

DC FieldValue Language
dc.contributor.authorRichmond, Craig J.en
dc.contributor.authorMatheu, Rocen
dc.contributor.authorPoater, Alberten
dc.contributor.authorFalivene, Lauraen
dc.contributor.authorBenet-Buchholz, Jordien
dc.contributor.authorSala, Xavieren
dc.contributor.authorCavallo, Luigien
dc.contributor.authorLlobet, Antoni A.en
dc.date.accessioned2015-08-03T12:16:43Zen
dc.date.available2015-08-03T12:16:43Zen
dc.date.issued2014-11-05en
dc.identifier.issn09476539en
dc.identifier.doi10.1002/chem.201405144en
dc.identifier.urihttp://hdl.handle.net/10754/563846en
dc.description.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.en
dc.description.sponsorshipC.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).en
dc.publisherWiley-Blackwellen
dc.subjectDFT calculationsen
dc.subjectRedox catalysisen
dc.subjectRutheniumen
dc.subjectSupramolecular chemistryen
dc.subjectWater splittingen
dc.titleSupramolecular water oxidation with rubda-based catalystsen
dc.typeArticleen
dc.contributor.departmentBiological and Environmental Sciences and Engineering (BESE) Divisionen
dc.contributor.departmentKAUST Catalysis Center (KCC)en
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentChemical Science Programen
dc.identifier.journalChemistry - A European Journalen
dc.contributor.institutionInstitute of Chemical Research of Catalonia (ICIQ), Av. Päisos Catalans 16Tarragona, Spainen
dc.contributor.institutionInstitut de Química Computacional i Catàlisi, Departament de Química, Universitat de GironaGirona, Spainen
dc.contributor.institutionDepartament de Química, Universitat Autonoma de Barcelona, Cerdanyola del VallèsBarcelona, Spainen
kaust.authorFalivene, Lauraen
kaust.authorCavallo, Luigien
dc.relation.isSupplementedByRichmond, 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/cc131bfxen
dc.relation.isSupplementedByDOI:10.5517/cc131bfxen
dc.relation.isSupplementedByHANDLE:http://hdl.handle.net/10754/624353en
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