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A robust molecular catalyst generated in situ for photo- and electrochemical water oxidation

Hussein A Younus, Nazir Ahmad, Adeel H Chughtai, Matthias Vandichel (UGent) , Michael Busch, Kristof Van Hecke (UGent) , Mekhman Yusubov, Shaoxian Song and Francis Verpoort (UGent)
(2017) CHEMSUSCHEM. 10(5). p.862-875
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Abstract
Water splitting is the key step towards artificial photosystems for solar energy conversion and storage in the form of chemical bonding. The oxidation of water is the bottle-neck of this process that hampers its practical utility; hence, efficient, robust, and easy to make catalytic systems based on cheap and earth-abundant materials are of exceptional importance. Herein, an in situ generated cobalt catalyst, [Co-II(TCA)(2)(H2O)(2)] (TCA=1-mesityl-1,2,3-1H-triazole-4-carboxylate), that efficiently conducts photochemical water oxidation under near-neutral conditions is presented. The catalyst showed high stability under photolytic conditions for more than 3 h of photoirradiation. During electrochemical water oxidation, the catalytic system assembled a catalyst film, which proved not to be cobalt oxide/hydroxide as normally expected, but instead, and for the first time, generated a molecular cobalt complex that incorporated the organic ligand bound to cobalt ions. The catalyst film exhibited a low overpotential for electrocatalytic water oxidation (360 mV) and high oxygen evolution peak current densities of 9 and 2.7 mA cm(-2) on glassy carbon and indium-doped tin oxide electrodes, respectively, at only 1.49 and 1.39 V ( versus a normal hydrogen electrode), respectively, under neutral conditions. This finding, exemplified on the in situ generated cobalt complex, might be applicable to other molecular systems and suggests that the formation of a catalytic film in electrochemical water oxidation experiments is not always an indication of catalyst decomposition and the formation of nanoparticles.
Keywords
cobalt, electrochemistry, oxidation, photochemistry, water splitting, OXYGEN EVOLUTION REACTION, MONONUCLEAR RUTHENIUM COMPLEXES, COBALT-POLYPYRIDINE COMPLEX, EVOLVING CATALYST, IRIDIUM COMPLEXES, PHOTOSYSTEM-II, HOMOGENEOUS CATALYSTS, IRON COMPLEXES, OXIDE SURFACES, VOLCANO PLOTS

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Citation

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MLA
Younus, Hussein A., et al. “A Robust Molecular Catalyst Generated in Situ for Photo- and Electrochemical Water Oxidation.” CHEMSUSCHEM, vol. 10, no. 5, 2017, pp. 862–75, doi:10.1002/cssc.201601477.
APA
Younus, H. A., Ahmad, N., Chughtai, A. H., Vandichel, M., Busch, M., Van Hecke, K., … Verpoort, F. (2017). A robust molecular catalyst generated in situ for photo- and electrochemical water oxidation. CHEMSUSCHEM, 10(5), 862–875. https://doi.org/10.1002/cssc.201601477
Chicago author-date
Younus, Hussein A, Nazir Ahmad, Adeel H Chughtai, Matthias Vandichel, Michael Busch, Kristof Van Hecke, Mekhman Yusubov, Shaoxian Song, and Francis Verpoort. 2017. “A Robust Molecular Catalyst Generated in Situ for Photo- and Electrochemical Water Oxidation.” CHEMSUSCHEM 10 (5): 862–75. https://doi.org/10.1002/cssc.201601477.
Chicago author-date (all authors)
Younus, Hussein A, Nazir Ahmad, Adeel H Chughtai, Matthias Vandichel, Michael Busch, Kristof Van Hecke, Mekhman Yusubov, Shaoxian Song, and Francis Verpoort. 2017. “A Robust Molecular Catalyst Generated in Situ for Photo- and Electrochemical Water Oxidation.” CHEMSUSCHEM 10 (5): 862–875. doi:10.1002/cssc.201601477.
Vancouver
1.
Younus HA, Ahmad N, Chughtai AH, Vandichel M, Busch M, Van Hecke K, et al. A robust molecular catalyst generated in situ for photo- and electrochemical water oxidation. CHEMSUSCHEM. 2017;10(5):862–75.
IEEE
[1]
H. A. Younus et al., “A robust molecular catalyst generated in situ for photo- and electrochemical water oxidation,” CHEMSUSCHEM, vol. 10, no. 5, pp. 862–875, 2017.
@article{8551389,
  abstract     = {{Water splitting is the key step towards artificial photosystems for solar energy conversion and storage in the form of chemical bonding. The oxidation of water is the bottle-neck of this process that hampers its practical utility; hence, efficient, robust, and easy to make catalytic systems based on cheap and earth-abundant materials are of exceptional importance. Herein, an in situ generated cobalt catalyst, [Co-II(TCA)(2)(H2O)(2)] (TCA=1-mesityl-1,2,3-1H-triazole-4-carboxylate), that efficiently conducts photochemical water oxidation under near-neutral conditions is presented. The catalyst showed high stability under photolytic conditions for more than 3 h of photoirradiation. During electrochemical water oxidation, the catalytic system assembled a catalyst film, which proved not to be cobalt oxide/hydroxide as normally expected, but instead, and for the first time, generated a molecular cobalt complex that incorporated the organic ligand bound to cobalt ions. The catalyst film exhibited a low overpotential for electrocatalytic water oxidation (360 mV) and high oxygen evolution peak current densities of 9 and 2.7 mA cm(-2) on glassy carbon and indium-doped tin oxide electrodes, respectively, at only 1.49 and 1.39 V ( versus a normal hydrogen electrode), respectively, under neutral conditions. This finding, exemplified on the in situ generated cobalt complex, might be applicable to other molecular systems and suggests that the formation of a catalytic film in electrochemical water oxidation experiments is not always an indication of catalyst decomposition and the formation of nanoparticles.}},
  author       = {{Younus, Hussein A and Ahmad, Nazir and Chughtai, Adeel H and Vandichel, Matthias and Busch, Michael and Van Hecke, Kristof and Yusubov, Mekhman and Song, Shaoxian and Verpoort, Francis}},
  issn         = {{1864-5631}},
  journal      = {{CHEMSUSCHEM}},
  keywords     = {{cobalt,electrochemistry,oxidation,photochemistry,water splitting,OXYGEN EVOLUTION REACTION,MONONUCLEAR RUTHENIUM COMPLEXES,COBALT-POLYPYRIDINE COMPLEX,EVOLVING CATALYST,IRIDIUM COMPLEXES,PHOTOSYSTEM-II,HOMOGENEOUS CATALYSTS,IRON COMPLEXES,OXIDE SURFACES,VOLCANO PLOTS}},
  language     = {{eng}},
  number       = {{5}},
  pages        = {{862--875}},
  title        = {{A robust molecular catalyst generated in situ for photo- and electrochemical water oxidation}},
  url          = {{http://doi.org/10.1002/cssc.201601477}},
  volume       = {{10}},
  year         = {{2017}},
}
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