Template-stabilized oxidic nickel oxygen evolution catalysts
Abstract
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.
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 https://www.pnas.org/lookup/suppl/doi:10.1073/pnas.2001529117/-/DCSupplemental.Attached Files
Published - 16187.full.pdf
Supplemental Material - pnas.2001529117.sapp.pdf
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Additional details
- PMCID
- PMC7368284
- Eprint ID
- 104267
- Resolver ID
- CaltechAUTHORS:20200708-071419168
- DE-SC0017619
- Department of Energy (DOE)
- NSF Graduate Research Fellowship
- Argonne National Laboratory
- Harvard University
- DE-AC02-06CH11357
- Department of Energy (DOE)
- ECS-0335765
- NSF
- Created
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2020-07-08Created from EPrint's datestamp field
- Updated
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2021-11-16Created from EPrint's last_modified field