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Title: In Silico Discovery of New Dopants for Fe-Doped Ni Oxyhydroxide (Ni1–xFexOOH) Catalysts for Oxygen Evolution Reaction

Abstract

The oxygen evolution reaction (OER) is critical to efficient water splitting to produce the H2 fuel for sustainable energy production. Currently, the best non-noble metal OER electrocatalyst in base conditions is the Fe-doped NiOOH (Ni1–xFexOOH), with an overpotential of η = 0.4, but much lower values are desired. We use density functional theory to determine the overall mechanism for the OER of Ni1–xFexOOH, concluding that promoting radical character on the metal–oxo bond is critical to efficient OER. Then we consider replacing Fe with 17 other transition metals of the Fe, Ru, and Os rows, where we find 3 new promising candidates: Co, Rh, and Ir, which we estimate to have η = 0.27, 0.15, and 0.02, respectively, all very much improved performance compared to Fe, making all three systems excellent candidates for experimental testing.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. California Inst. of Technology (CalTech), Pasadena, CA (United States)
Publication Date:
Research Org.:
California Institute of Technology (CalTech), Pasadena, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1467620
Grant/Contract Number:  
SC0004993
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 140; Journal Issue: 22; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Shin, Hyeyoung, Xiao, Hai, and Goddard, III, William A. In Silico Discovery of New Dopants for Fe-Doped Ni Oxyhydroxide (Ni1–xFexOOH) Catalysts for Oxygen Evolution Reaction. United States: N. p., 2018. Web. doi:10.1021/jacs.8b02225.
Shin, Hyeyoung, Xiao, Hai, & Goddard, III, William A. In Silico Discovery of New Dopants for Fe-Doped Ni Oxyhydroxide (Ni1–xFexOOH) Catalysts for Oxygen Evolution Reaction. United States. https://doi.org/10.1021/jacs.8b02225
Shin, Hyeyoung, Xiao, Hai, and Goddard, III, William A. Fri . "In Silico Discovery of New Dopants for Fe-Doped Ni Oxyhydroxide (Ni1–xFexOOH) Catalysts for Oxygen Evolution Reaction". United States. https://doi.org/10.1021/jacs.8b02225. https://www.osti.gov/servlets/purl/1467620.
@article{osti_1467620,
title = {In Silico Discovery of New Dopants for Fe-Doped Ni Oxyhydroxide (Ni1–xFexOOH) Catalysts for Oxygen Evolution Reaction},
author = {Shin, Hyeyoung and Xiao, Hai and Goddard, III, William A.},
abstractNote = {The oxygen evolution reaction (OER) is critical to efficient water splitting to produce the H2 fuel for sustainable energy production. Currently, the best non-noble metal OER electrocatalyst in base conditions is the Fe-doped NiOOH (Ni1–xFexOOH), with an overpotential of η = 0.4, but much lower values are desired. We use density functional theory to determine the overall mechanism for the OER of Ni1–xFexOOH, concluding that promoting radical character on the metal–oxo bond is critical to efficient OER. Then we consider replacing Fe with 17 other transition metals of the Fe, Ru, and Os rows, where we find 3 new promising candidates: Co, Rh, and Ir, which we estimate to have η = 0.27, 0.15, and 0.02, respectively, all very much improved performance compared to Fe, making all three systems excellent candidates for experimental testing.},
doi = {10.1021/jacs.8b02225},
journal = {Journal of the American Chemical Society},
number = 22,
volume = 140,
place = {United States},
year = {2018},
month = {5}
}

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Cited by: 248 works
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Figures / Tables:

Figure 1 Figure 1: Models for NiOOH and Ni1-xFexOOH OER electrocatalysts. (100) slab models with one explicit water layer for (a) γ-NiOOH and (b) γ-Ni1-xFexOOH. Blue, purple, red, white, green and gray atoms indicate Ni4+, Ni3+, O, H, K+, and Fe4+, respectively. Chemical structures for each model surface are shown as insets.more » (Note that the intercalating K+ and H2O are not shown in the insets for clarity.)« less

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.