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Domain Structures of Ni and NiFe (Oxy)Hydroxide Oxygen-Evolution Catalysts from X-ray Pair Distribution Function Analysis
Abstract
Ni-Fe (oxy)hydroxides, Ni(i-z)FezOxHy, are among the fastest-known water oxidation catalysts in alkaline media on a per-cation basis. At current densities relevant for electrolysis (e.g., >0.5 A/cm(-2)), mass and electron transport through catalyst films with high mass loading are critical and depend substantially on the extended and intermediate catalyst architecture. We use X-ray pair distribution function (PDF) analysis to determine the intermediate nanostructures of electrodeposited Ni(i-z)FezOxHy films. We report the effects of electrodeposition technique (pulsed versus continuous), electrochemical cycling, and Fe content on the structure of the catalyst film. The PDF patterns for Ni(i-z)FezOxHy films are best simulated by model structures consisting of brucite-like β-Ni(OH)2 fragments 1 to 3 layers in thickness. Only the oxidation state of the film significantly affects the intralayer scattering behavior (i.e., metal-oxygen bond distance). The interlayer interactions, however, are affected by Fe content and deposition conditions. The domain size of many of the systems are similar, extending to similar to ~5 nm, which are best modeled by sheets containing upward of similar to ~250 metal cations. Smaller domains were found for films deposited through a larger number of electrochemical cathodic current pulses. Films can be cycled between as-deposited, oxidized, and reduced states, with minimal loss ofmore »
- Authors:
-
[1]
- Univ. of Oregon, Eugene, OR (United States). Dept. of Chemistry
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS) and Chemical Sciences and Engineering Division
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF); US Air Force Academy; Sloan Foundation; Dreyfus Foundation; W. M. Keck Foundation; M. J. Murdock Charitable Trust; Air Force Research Laboratory (AFRL)
- OSTI Identifier:
- 1461297
- Grant/Contract Number:
- AC02-06CH11357; CHE-1566348; SC0001059
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 121; Journal Issue: 45; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE
Citation Formats
Batchellor, Adam S., Kwon, Gihan, Laskowski, Forrest A. L., Tiede, David M., and Boettcher, Shannon W. Domain Structures of Ni and NiFe (Oxy)Hydroxide Oxygen-Evolution Catalysts from X-ray Pair Distribution Function Analysis. United States: N. p., 2017.
Web. doi:10.1021/acs.jpcc.7b10306.
Batchellor, Adam S., Kwon, Gihan, Laskowski, Forrest A. L., Tiede, David M., & Boettcher, Shannon W. Domain Structures of Ni and NiFe (Oxy)Hydroxide Oxygen-Evolution Catalysts from X-ray Pair Distribution Function Analysis. United States. https://doi.org/10.1021/acs.jpcc.7b10306
Batchellor, Adam S., Kwon, Gihan, Laskowski, Forrest A. L., Tiede, David M., and Boettcher, Shannon W. 2017.
"Domain Structures of Ni and NiFe (Oxy)Hydroxide Oxygen-Evolution Catalysts from X-ray Pair Distribution Function Analysis". United States. https://doi.org/10.1021/acs.jpcc.7b10306. https://www.osti.gov/servlets/purl/1461297.
@article{osti_1461297,
title = {Domain Structures of Ni and NiFe (Oxy)Hydroxide Oxygen-Evolution Catalysts from X-ray Pair Distribution Function Analysis},
author = {Batchellor, Adam S. and Kwon, Gihan and Laskowski, Forrest A. L. and Tiede, David M. and Boettcher, Shannon W.},
abstractNote = {Ni-Fe (oxy)hydroxides, Ni(i-z)FezOxHy, are among the fastest-known water oxidation catalysts in alkaline media on a per-cation basis. At current densities relevant for electrolysis (e.g., >0.5 A/cm(-2)), mass and electron transport through catalyst films with high mass loading are critical and depend substantially on the extended and intermediate catalyst architecture. We use X-ray pair distribution function (PDF) analysis to determine the intermediate nanostructures of electrodeposited Ni(i-z)FezOxHy films. We report the effects of electrodeposition technique (pulsed versus continuous), electrochemical cycling, and Fe content on the structure of the catalyst film. The PDF patterns for Ni(i-z)FezOxHy films are best simulated by model structures consisting of brucite-like β-Ni(OH)2 fragments 1 to 3 layers in thickness. Only the oxidation state of the film significantly affects the intralayer scattering behavior (i.e., metal-oxygen bond distance). The interlayer interactions, however, are affected by Fe content and deposition conditions. The domain size of many of the systems are similar, extending to similar to ~5 nm, which are best modeled by sheets containing upward of similar to ~250 metal cations. Smaller domains were found for films deposited through a larger number of electrochemical cathodic current pulses. Films can be cycled between as-deposited, oxidized, and reduced states, with minimal loss of intrasheet coherence, indicating a degree of structural stability. We estimate heterogeneity in the domain structures by modeling the PDF data to linear combinations of oxyhydroxide fragments with different sizes and numbers of layers.},
doi = {10.1021/acs.jpcc.7b10306},
url = {https://www.osti.gov/biblio/1461297},
journal = {Journal of Physical Chemistry. C},
issn = {1932-7447},
number = 45,
volume = 121,
place = {United States},
year = {Fri Oct 20 00:00:00 EDT 2017},
month = {Fri Oct 20 00:00:00 EDT 2017}
}
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