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Title: Theoretical Insights to Bulk Activity Towards Oxygen Evolution in Oxyhydroxides

The nature of the electrochemical water splitting activity of layered pure and Fe-doped NiOOH is investigated using density functional theory calculations. We find similar thermodynamics for the oxygen evolution reaction (OER) intermediates between the layers of oxyhydroxides, that is, in the bulk of the materials as on the (001) surface. The effect of interlayer spacing on adsorption energy is affected by both the crystal structure and the level of hydrogenation of the active sites. For the Fe-doped NiOOH, we observe general weakening of binding between the different OER intermediates and the catalyst material. The calculated OER activity depends both on doping and interlayer spacing, and our results are generally congruent with available experimental data. In conclusion, these results suggest that such interlayer “bulk” sites may contribute to measured OER activity for both the pure and Fe-doped NiOOH catalysts.
Authors:
 [1] ;  [2] ; ORCiD logo [3]
  1. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  3. Univ. of Pennsylvania, Philadelphia, PA (United States)
Publication Date:
Grant/Contract Number:
AC02-76SF00515; SUNCAT Center for Interface Science and Catalysis; Laboratory-Directed Research and Development progr
Type:
Accepted Manuscript
Journal Name:
Catalysis Letters
Additional Journal Information:
Journal Volume: 147; Journal Issue: 6; Journal ID: ISSN 1011-372X
Publisher:
Springer
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Oxygen evolution; Oxyhydroxide; Electrolysis; Electrocatalysis
OSTI Identifier:
1367845

Doyle, Andrew D., Bajdich, Michal, and Vojvodic, Aleksandra. Theoretical Insights to Bulk Activity Towards Oxygen Evolution in Oxyhydroxides. United States: N. p., Web. doi:10.1007/s10562-017-2010-z.
Doyle, Andrew D., Bajdich, Michal, & Vojvodic, Aleksandra. Theoretical Insights to Bulk Activity Towards Oxygen Evolution in Oxyhydroxides. United States. doi:10.1007/s10562-017-2010-z.
Doyle, Andrew D., Bajdich, Michal, and Vojvodic, Aleksandra. 2017. "Theoretical Insights to Bulk Activity Towards Oxygen Evolution in Oxyhydroxides". United States. doi:10.1007/s10562-017-2010-z. https://www.osti.gov/servlets/purl/1367845.
@article{osti_1367845,
title = {Theoretical Insights to Bulk Activity Towards Oxygen Evolution in Oxyhydroxides},
author = {Doyle, Andrew D. and Bajdich, Michal and Vojvodic, Aleksandra},
abstractNote = {The nature of the electrochemical water splitting activity of layered pure and Fe-doped NiOOH is investigated using density functional theory calculations. We find similar thermodynamics for the oxygen evolution reaction (OER) intermediates between the layers of oxyhydroxides, that is, in the bulk of the materials as on the (001) surface. The effect of interlayer spacing on adsorption energy is affected by both the crystal structure and the level of hydrogenation of the active sites. For the Fe-doped NiOOH, we observe general weakening of binding between the different OER intermediates and the catalyst material. The calculated OER activity depends both on doping and interlayer spacing, and our results are generally congruent with available experimental data. In conclusion, these results suggest that such interlayer “bulk” sites may contribute to measured OER activity for both the pure and Fe-doped NiOOH catalysts.},
doi = {10.1007/s10562-017-2010-z},
journal = {Catalysis Letters},
number = 6,
volume = 147,
place = {United States},
year = {2017},
month = {4}
}

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