A molecular catalyst for water oxidation that binds to metal oxide surfaces
Abstract
Here, 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.
- Authors:
-
- Yale Univ., New Haven, CT (United States)
- Yale Univ., New Haven, CT (United States); Univ. of Bath (United Kingdom)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research Center (ANSER); Energy Frontier Research Centers (EFRC) (United States). Center for Catalytic Hydrocarbon Functionalization (CCHF)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1210447
- Grant/Contract Number:
- SC0001059
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 6; Journal Issue: 1; Related Information: ANSER partners with Northwestern University (lead); Argonne National Laboratory; University of Chicago; University of Illinois, Urbana-Champaign; Yale University; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (homogeneous); catalysis (heterogeneous); solar (photovoltaic); solar (fuels); photosynthesis (natural and artificial); bio-inspired; hydrogen and fuel cells; electrodes - solar; defects; charge transport; spin dynamics; membrane; materials and chemistry by design; optics; synthesis (novel materials); synthesis (self-assembly)
Citation Formats
Sheehan, Stafford W., Thomsen, Julianne M., Hintermair, Ulrich, Crabtree, Robert H., Brudvig, Gary W., and Schmuttenmaer, Charles A. A molecular catalyst for water oxidation that binds to metal oxide surfaces. United States: N. p., 2015.
Web. doi:10.1038/ncomms7469.
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. United States. https://doi.org/10.1038/ncomms7469
Sheehan, Stafford W., Thomsen, Julianne M., Hintermair, Ulrich, Crabtree, Robert H., Brudvig, Gary W., and Schmuttenmaer, Charles A. Wed .
"A molecular catalyst for water oxidation that binds to metal oxide surfaces". United States. https://doi.org/10.1038/ncomms7469. https://www.osti.gov/servlets/purl/1210447.
@article{osti_1210447,
title = {A molecular catalyst for water oxidation that binds to metal oxide surfaces},
author = {Sheehan, Stafford W. and Thomsen, Julianne M. and Hintermair, Ulrich and Crabtree, Robert H. and Brudvig, Gary W. and Schmuttenmaer, Charles A.},
abstractNote = {Here, 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.},
doi = {10.1038/ncomms7469},
journal = {Nature Communications},
number = 1,
volume = 6,
place = {United States},
year = {Wed Mar 11 00:00:00 EDT 2015},
month = {Wed Mar 11 00:00:00 EDT 2015}
}
Web of Science
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A molecular ruthenium catalyst with water-oxidation activity comparable to that of photosystem II
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A soluble copper–bipyridine water-oxidation electrocatalyst
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Photocatalytic water oxidation with cobalt-containing tungstobismutates: tuning the metal core
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- Vannucci, A. K.; Alibabaei, L.; Losego, M. D.
- Proceedings of the National Academy of Sciences, Vol. 110, Issue 52
Homogeneous Catalysis--New Approaches to Catalyst Separation, Recovery, and Recycling
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- Cole-Hamilton, David J.
- Science, Vol. 299, Issue 5613, p. 1702-1706
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