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A molecular catalyst for water oxidation that binds to metal oxide surfaces

Molecular catalysts are known for their high activity and tunability, but their solubility and limited stability often restrict their use in practical applications. Here we describe how a molecular iridium catalyst for water oxidation directly and robustly binds to oxide surfaces without the need fo...

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Autores principales: Sheehan, Stafford W., Thomsen, Julianne M., Hintermair, Ulrich, Crabtree, Robert H., Brudvig, Gary W., Schmuttenmaer, Charles A.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Pub. Group 2015
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4382695/
https://www.ncbi.nlm.nih.gov/pubmed/25757425
http://dx.doi.org/10.1038/ncomms7469
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author Sheehan, Stafford W.
Thomsen, Julianne M.
Hintermair, Ulrich
Crabtree, Robert H.
Brudvig, Gary W.
Schmuttenmaer, Charles A.
author_facet Sheehan, Stafford W.
Thomsen, Julianne M.
Hintermair, Ulrich
Crabtree, Robert H.
Brudvig, Gary W.
Schmuttenmaer, Charles A.
author_sort Sheehan, Stafford W.
collection PubMed
description Molecular catalysts are known for their high activity and tunability, but their solubility and limited stability often restrict their use in practical applications. Here we describe how a molecular iridium catalyst for water oxidation directly and robustly binds to oxide surfaces without the need for any external stimulus or additional linking groups. On conductive electrode surfaces, this heterogenized molecular catalyst oxidizes water with low overpotential, high turnover frequency and minimal degradation. Spectroscopic and electrochemical studies show that it does not decompose into iridium oxide, thus preserving its molecular identity, and that it is capable of sustaining high activity towards water oxidation with stability comparable to state-of-the-art bulk metal oxide catalysts.
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spelling pubmed-43826952015-04-07 A molecular catalyst for water oxidation that binds to metal oxide surfaces Sheehan, Stafford W. Thomsen, Julianne M. Hintermair, Ulrich Crabtree, Robert H. Brudvig, Gary W. Schmuttenmaer, Charles A. Nat Commun Article Molecular catalysts are known for their high activity and tunability, but their solubility and limited stability often restrict their use in practical applications. Here we describe how a molecular iridium catalyst for water oxidation directly and robustly binds to oxide surfaces without the need for any external stimulus or additional linking groups. On conductive electrode surfaces, this heterogenized molecular catalyst oxidizes water with low overpotential, high turnover frequency and minimal degradation. Spectroscopic and electrochemical studies show that it does not decompose into iridium oxide, thus preserving its molecular identity, and that it is capable of sustaining high activity towards water oxidation with stability comparable to state-of-the-art bulk metal oxide catalysts. Nature Pub. Group 2015-03-11 /pmc/articles/PMC4382695/ /pubmed/25757425 http://dx.doi.org/10.1038/ncomms7469 Text en Copyright © 2015, Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved. http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
spellingShingle Article
Sheehan, Stafford W.
Thomsen, Julianne M.
Hintermair, Ulrich
Crabtree, Robert H.
Brudvig, Gary W.
Schmuttenmaer, Charles A.
A molecular catalyst for water oxidation that binds to metal oxide surfaces
title A molecular catalyst for water oxidation that binds to metal oxide surfaces
title_full A molecular catalyst for water oxidation that binds to metal oxide surfaces
title_fullStr A molecular catalyst for water oxidation that binds to metal oxide surfaces
title_full_unstemmed A molecular catalyst for water oxidation that binds to metal oxide surfaces
title_short A molecular catalyst for water oxidation that binds to metal oxide surfaces
title_sort molecular catalyst for water oxidation that binds to metal oxide surfaces
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4382695/
https://www.ncbi.nlm.nih.gov/pubmed/25757425
http://dx.doi.org/10.1038/ncomms7469
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