A Robust Molecular Catalyst Generated In?Situ for Photo- and Electrochemical Water Oxidation
| Parent link: | ChemSusChem Vol. 10, iss. 5.— 2017.— [P. 862-875] |
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| Corporate Author: | |
| Other Authors: | , , , , , , , , |
| Summary: | Title screen 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, [CoII(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. |
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2017
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| Online Access: | http://dx.doi.org/10.1002/cssc.201601477 |
| Format: | Electronic Book Chapter |
| KOHA link: | https://koha.lib.tpu.ru/cgi-bin/koha/opac-detail.pl?biblionumber=656171 |