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Incorporation of Hydrogen-Bonding Functionalities into the Second Coordination Sphere of Iron-Based Water-Oxidation Catalysts

Hoffert, Wesley A. and Mock, Michael T. and Appel, Aaron M. and Yang, Jenny Y. (2013) Incorporation of Hydrogen-Bonding Functionalities into the Second Coordination Sphere of Iron-Based Water-Oxidation Catalysts. European Journal of Inorganic Chemistry, 2013 (22-23). pp. 3846-3857. ISSN 1434-1948. doi:10.1002/ejic.201201499. https://resolver.caltech.edu/CaltechAUTHORS:20140206-140835683

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Abstract

Energy storage and conversion schemes based on environmentally benign chemical fuels will require the discovery of faster, cheaper, and more robust catalysts for the oxygen-evolution reaction (OER). Although the incorporation of pendant bases into molecular catalysts for hydrogen production and utilization has led to enhanced turnover frequencies, the analogous incorporation of pendant bases into molecular catalysts for water oxidation has received little attention. Herein, the syntheses, structures, and catalytic activities of new iron complexes with pendant bases are reported. Of these new complexes, [Fe(L^1)]^(2+) {L^1 = N,N′-dimethyl-N,N′-bis(pyridazin-3-ylmethyl)ethane-1,2-diamine} is the most active catalyst. Initial turnover frequencies of 141 and 24 h^(–1) were measured by using ceric ammonium nitrate at pH 0.7 and sodium periodate at pH 4.7, respectively. These results suggest that the incorporation of pendant bases into molecular catalysts for water oxidation might be an effective strategy that can be considered in the development of new catalysts for the OER, but will require the careful balance of many factors.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1002/ejic.201201499DOIArticle
http://onlinelibrary.wiley.com/doi/10.1002/ejic.201201499/abstractPublisherArticle
Additional Information:© 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. Received: December 12, 2012; Published Online: April 9, 2013. This work was supported by the Laboratory Directed Research and Development program at Pacific Northwest National Laboratory (PNNL). M. T. M. was supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. PNNL is operated by Battelle for the US Department of Energy.
Funders:
Funding AgencyGrant Number
Pacific Northwest National Laboratory (PNNL) Laboratory Directed Research and Development programUNSPECIFIED
Center for Molecular ElectrocatalysisUNSPECIFIED
Subject Keywords:Homogeneous catalysis; Water splitting; Iron; Ligand effects; Proton transport
Issue or Number:22-23
DOI:10.1002/ejic.201201499
Record Number:CaltechAUTHORS:20140206-140835683
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20140206-140835683
Official Citation:Hoffert, W. A., Mock, M. T., Appel, A. M., & Yang, J. Y. (2013). Incorporation of Hydrogen-Bonding Functionalities into the Second Coordination Sphere of Iron-Based Water-Oxidation Catalysts. European Journal of Inorganic Chemistry, 2013(22-23), 3846-3857. doi: 10.1002/ejic.201201499
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:43706
Collection:CaltechAUTHORS
Deposited By: Bianca Rios
Deposited On:07 Feb 2014 00:00
Last Modified:10 Nov 2021 16:41

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