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Title: 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:
 [1];  [1];  [2];  [1];  [1];  [1]
  1. Yale Univ., New Haven, CT (United States)
  2. Yale Univ., New Haven, CT (United States); Univ. of Bath (United Kingdom)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC), Washington, D.C. (United States); Argonne-Northwestern Solar Energy Research Center (ANSER)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1210447
Grant/Contract Number:  
SC0001059
Resource Type:
Journal Article: 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. doi: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. doi: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}
}

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Cited by: 89 works
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