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Template-stabilized oxidic nickel oxygen evolution catalysts

Li, Nancy and Keane, Thomas P. and Veroneau, Samuel S. and Hadt, Ryan G. and Hayes, Dugan and Chen, Lin X. and Nocera, Daniel G. (2020) Template-stabilized oxidic nickel oxygen evolution catalysts. Proceedings of the National Academy of Sciences of the United States of America, 117 (28). pp. 16187-16192. ISSN 0027-8424. PMCID PMC7368284. doi:10.1073/pnas.2001529117.

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Earth-abundant oxygen evolution catalysts (OECs) with extended stability in acid can be constructed by embedding active sites within an acid-stable metal-oxide framework. Here, we report stable NiPbO_x films that are able to perform oxygen evolution reaction (OER) catalysis for extended periods of operation (>20 h) in acidic solutions of pH 2.5; conversely, native NiO_x catalyst films dissolve immediately. In situ X-ray absorption spectroscopy and ex situ X-ray photoelectron spectroscopy reveal that PbO₂ is unperturbed after addition of Ni and/or Fe into the lattice, which serves as an acid-stable, conductive framework for embedded OER active centers. The ability to perform OER in acid allows the mechanism of Fe doping on Ni catalysts to be further probed. Catalyst activity with Fe doping of oxidic Ni OEC under acid conditions, as compared to neutral or basic conditions, supports the contention that role of Fe³⁺ in enhancing catalytic activity in Ni oxide catalysts arises from its Lewis acid properties.

Item Type:Article
Related URLs:
URLURL TypeDescription Information CentralArticle
Hadt, Ryan G.0000-0001-6026-1358
Hayes, Dugan0000-0003-4171-5179
Chen, Lin X.0000-0002-8450-6687
Nocera, Daniel G.0000-0001-5055-320X
Additional Information:© 2020 National Academy of Sciences. Published under the PNAS license. Contributed by Daniel G. Nocera, May 29, 2020 (sent for review January 27, 2020; reviewed by Curtis P. Berlinguette and Xile Hu). PNAS first published July 7, 2020. Material is based on work supported under the Solar Photochemistry Program of the Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences of the US Department of Energy Grant DE-SC0017619. We thank Joe Elias for assistance with XPS and Tuncay Ozel for help with SEM and Michael Huynh and David Gygi for helpful discussions. T.P.K. acknowledges support from a Graduate Research Fellowship from the NSF. R.G.H. acknowledges support from an Enrico Fermi Fellowship at Argonne National Laboratory (ANL). S.S.V acknowledges support from the Herchel Smith Graduate Fellowship in the Sciences. D.H. acknowledges support from a Joseph J. Katz Fellowship at ANL. L.X.C. acknowledges the support from Chemical, Biological and Geological Sciences, Basic Energy Sciences, Office of Science, Office of Basic Energy Sciences, under Contract DE-AC02-06CH11357. SEM and XPS were performed at Harvard University’s Center for Nanoscale Systems, a member of the National Nanotechnology Infrastructure Network, which is supported by the NSF under ECS-0335765. Use of beamline 12BM-B at the Advanced Photon Source at Argonne National Laboratory was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract DE-AC02-06CH11357. Author contributions: N.L., T.P.K., S.S.V., R.G.H., D.H., L.X.C., and D.G.N. designed research; N.L., T.P.K., S.S.V., R.G.H., and D.H. performed research; N.L., T.P.K., S.S.V., R.G.H., and D.H. contributed new reagents/analytic tools; N.L., T.P.K., S.S.V., R.G.H., D.H., L.X.C., and D.G.N. analyzed data; and N.L., T.P.K., S.S.V., and D.G.N. wrote the paper. Reviewers: C.P.B., University of British Columbia; and X.H., EPFL, Lausanne. The authors declare no competing interest. This article contains supporting information online at
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0017619
NSF Graduate Research FellowshipUNSPECIFIED
Argonne National LaboratoryUNSPECIFIED
Harvard UniversityUNSPECIFIED
Department of Energy (DOE)DE-AC02-06CH11357
Subject Keywords:water-splitting catalysis; renewable energy; solar to fuels; electrocatalysis; acid-stable templating
Issue or Number:28
PubMed Central ID:PMC7368284
Record Number:CaltechAUTHORS:20200708-071419168
Persistent URL:
Official Citation:Template-stabilized oxidic nickel oxygen evolution catalysts. Nancy Li, Thomas P. Keane, Samuel S. Veroneau, Ryan G. Hadt, Dugan Hayes, Lin X. Chen, Daniel G. Nocera. Proceedings of the National Academy of Sciences Jul 2020, 117 (28) 16187-16192; DOI: 10.1073/pnas.2001529117
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:104267
Deposited By: Tony Diaz
Deposited On:08 Jul 2020 15:42
Last Modified:16 Nov 2021 18:30

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