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

doi:10.1002/chem.201405144

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 journal › Article › peer-review

75 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 language	English (US)
Pages (from-to)	17282-17286
Number of pages	5
Journal	Chemistry - A European Journal
Volume	20
Issue number	52
DOIs	https://doi.org/10.1002/chem.201405144
State	Published - 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

General Chemistry

Access to Document

10.1002/chem.201405144

https://repository.kaust.edu.sa/bitstream/10754/563846/1/OA-Supramolecular%20Water%20Oxidation%20with%20Ru-bda%20Based%20Catalysts.pdf

Cite this

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title = "Supramolecular water oxidation with rubda-based catalysts",

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.",

author = "Richmond, {Craig J.} and Roc Matheu and Albert Poater and Laura Falivene and Jordi Benet-Buchholz and Xavier Sala and Luigi Cavallo and Llobet, {Antoni A.}",

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).",

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AU - Richmond, Craig J.

AU - Matheu, Roc

AU - Poater, Albert

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AU - Sala, Xavier

AU - Cavallo, Luigi

AU - Llobet, Antoni A.

N1 - 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).

PY - 2014/11/5

Y1 - 2014/11/5

N2 - 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.

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Supramolecular water oxidation with rubda-based catalysts

Abstract

Bibliographical note

ASJC Scopus subject areas

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CCDC 1014178: Experimental Crystal Structure Determination : (2,2'-bipyridine-6,6'-dicarboxylato)-bis(6-methoxyisoquinoline)-ruthenium methanol solvate trihydrate

Cite this

Supramolecular water oxidation with rubda-based catalysts

Abstract

Bibliographical note

ASJC Scopus subject areas

Access to Document

Other files and links

Fingerprint

Datasets

CCDC 1014178: Experimental Crystal Structure Determination : (2,2'-bipyridine-6,6'-dicarboxylato)-bis(6-methoxyisoquinoline)-ruthenium methanol solvate trihydrate

Cite this