Domain Structures of Ni and NiFe (Oxy)Hydroxide Oxygen-Evolution Catalysts from X-ray Pair Distribution Function Analysis

Batchellor, Adam S.; Kwon, Gihan; Laskowski, Forrest A.  L.; Tiede, David M.; Boettcher, Shannon W.

doi:10.1021/acs.jpcc.7b10306

Title: Domain Structures of Ni and NiFe (Oxy)Hydroxide Oxygen-Evolution Catalysts from X-ray Pair Distribution Function Analysis

Journal Article · 20 October 2017 · Journal of Physical Chemistry. C

DOI: https://doi.org/10.1021/acs.jpcc.7b10306 · OSTI ID:1461297

Batchellor, Adam S. ^[1]; Kwon, Gihan ^[2]; Laskowski, Forrest A. L. ^[1]; Tiede, David M. ^[2];

^[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

Ni-Fe (oxy)hydroxides, Ni(_i-z)Fe_zO_xH_y, 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)Fe_zO_xH_y 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)Fe_zO_xH_y 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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: 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)

Grant/Contract Number:: AC02-06CH11357; CHE-1566348; SC0001059

OSTI ID:: 1461297

Journal Information:: Journal of Physical Chemistry. C, Vol. 121, Issue 45; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 22 works

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