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Effect of interlayer anions on [NiFe]-LDH nanosheet water oxidation activity

Hunter, B. M. and Hieringer, W. and Winkler, J. R. and Gray, H. B. and Müller, A. M. (2016) Effect of interlayer anions on [NiFe]-LDH nanosheet water oxidation activity. Energy and Environmental Science, 2016 (5). pp. 1734-1743. ISSN 1754-5692. doi:10.1039/C6EE00377J.

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We synthesized nickel–iron layered double hydroxide ([NiFe]-LDH) nanosheets with different interlayer anions to probe their role in water oxidation catalysis. In alkaline electrolyte in ambient air, carbonate rapidly replaced other interlayer anions and catalytic activity was highest. Electrocatalytic water oxidation in virtually carbonate-free alkaline electrolyte revealed that activity was a function of anion basicity. Our [NiFe]-LDH nanosheets, prepared by pulsed laser ablation in liquids, were regenerated in carbonate-containing aqueous KOH. Anion binding motifs were assessed by X-ray photoelectron spectroscopy in combination with density functional theory calculations, suggesting that nitrite species bound to edge-site Fe in the precatalyst correlated with higher water oxidation activity.

Item Type:Article
Related URLs:
URLURL TypeDescription Information
Hunter, B. M.0000-0001-8559-9304
Winkler, J. R.0000-0002-4453-9716
Gray, H. B.0000-0002-7937-7876
Müller, A. M.0000-0002-2785-6808
Additional Information:© 2016 Royal Society of Chemistry. Received 5th February 2016, Accepted 17th March 2016. First published online 17 Mar 2016. We thank George Rossman for help with solid-state IR spectroscopy. Research was carried out in the Laser Resource Center and the Molecular Materials Research Center of the Beckman Institute of the California Institute of Technology. This work was supported by the NSF CCI Solar Fuels Program (CHE-1305124) and the Arnold and Mabel Beckman Foundation. B. M. H. is a Fellow of the Resnick Sustainability Institute at Caltech. W. H. thanks the Deutsche Forschungsgemeinschaft and the Cluster of Excellence "Engineering of Advanced Materials" at the University of Erlangen-Nürnberg for support.
Group:CCI Solar Fuels, Resnick Sustainability Institute
Funding AgencyGrant Number
Arnold and Mabel Beckman FoundationUNSPECIFIED
Resnick Sustainability InstituteUNSPECIFIED
Deutsche Forschungsgemeinschaft (DFG)UNSPECIFIED
University of Erlangen-NürnbergUNSPECIFIED
Issue or Number:5
Record Number:CaltechAUTHORS:20160404-081907582
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Official Citation:Effect of interlayer anions on [NiFe]-LDH nanosheet water oxidation activity B. M. Hunter, W. Hieringer, J. R. Winkler, H. B. Gray and A. M. Müller Energy Environ. Sci., 2016,9, 1734-1743 DOI: 10.1039/C6EE00377J
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:65876
Deposited By: Ruth Sustaita
Deposited On:04 Apr 2016 19:13
Last Modified:10 Nov 2021 23:50

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