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

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 Llobet

Research output: Contribution to journal › Article › Research › peer-review

57 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 language	English
Pages (from-to)	17282-17286
Journal	Chemistry - A European Journal
Volume	20
Issue number	52
DOIs	https://doi.org/10.1002/chem.201405144
Publication status	Published - 22 Dec 2014

Keywords

DFT calculations
Redox catalysis
Ruthenium
Supramolecular chemistry
Water splitting

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

abstract = "{\textcopyright} 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.",

keywords = "DFT calculations, Redox catalysis, Ruthenium, Supramolecular chemistry, Water splitting",

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

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T1 - Supramolecular water oxidation with rubda-based catalysts

AU - Richmond, Craig J.

AU - Matheu, Roc

AU - Poater, Albert

AU - Falivene, Laura

AU - Benet-Buchholz, Jordi

AU - Sala, Xavier

AU - Cavallo, Luigi

AU - Llobet, Antoni

PY - 2014/12/22

Y1 - 2014/12/22

N2 - © 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.

AB - © 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.

KW - DFT calculations

KW - Redox catalysis

KW - Ruthenium

KW - Supramolecular chemistry

KW - Water splitting

U2 - 10.1002/chem.201405144

DO - 10.1002/chem.201405144

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