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Title: Water electrolysis on La 1-xSr xCoO 3-δ perovskite electrocatalysts

Abstract

Here, perovskite oxides are attractive candidates as catalysts for the electrolysis of water in alkaline energy storage and conversion systems. However, the rational design of active catalysts has been hampered by the lack of understanding of the mechanism of water electrolysis on perovskite surfaces. Key parameters that have been overlooked include the role of oxygen vacancies, B–O bond covalency, and redox activity of lattice oxygen species. Here we present a series of cobaltite perovskites where the covalency of the Co–O bond and the concentration of oxygen vacancies are controlled through Sr 2+ substitution into La 1–xSr xCoO 3–δ. We attempt to rationalize the high activities of La 1–xSr xCoO 3–δ through the electronic structure and participation of lattice oxygen in the mechanism of water electrolysis as revealed through ab initio modelling. Using this approach, we report a material, SrCoO 2.7, with a high, room temperature-specific activity and mass activity towards alkaline water electrolysis.

Authors:
 [1];  [2];  [3];  [1];  [4];  [2];  [1];  [5]
  1. Univ. of Texas at Austin, Austin, TX (United States)
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  3. Skolkovo Institute of Science and Technology, Moscow (Russia); Univ. of Antwerp, Antwerp (Belgium)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  5. Univ. of Texas at Austin, Austin, TX (United States); Skolkovo Institute of Science and Technology, Moscow (Russia)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1261341
Alternate Identifier(s):
OSTI ID: 1324110
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Mefford, J. Tyler, Rong, Xi, Abakumov, Artem M., Hardin, William G., Dai, Sheng, Kolpak, Alexie, Johnston, Keith P., and Stevenson, Keith J. Water electrolysis on La1-xSrxCoO3-δ perovskite electrocatalysts. United States: N. p., 2016. Web. doi:10.1038/ncomms11053.
Mefford, J. Tyler, Rong, Xi, Abakumov, Artem M., Hardin, William G., Dai, Sheng, Kolpak, Alexie, Johnston, Keith P., & Stevenson, Keith J. Water electrolysis on La1-xSrxCoO3-δ perovskite electrocatalysts. United States. doi:10.1038/ncomms11053.
Mefford, J. Tyler, Rong, Xi, Abakumov, Artem M., Hardin, William G., Dai, Sheng, Kolpak, Alexie, Johnston, Keith P., and Stevenson, Keith J. Wed . "Water electrolysis on La1-xSrxCoO3-δ perovskite electrocatalysts". United States. doi:10.1038/ncomms11053. https://www.osti.gov/servlets/purl/1261341.
@article{osti_1261341,
title = {Water electrolysis on La1-xSrxCoO3-δ perovskite electrocatalysts},
author = {Mefford, J. Tyler and Rong, Xi and Abakumov, Artem M. and Hardin, William G. and Dai, Sheng and Kolpak, Alexie and Johnston, Keith P. and Stevenson, Keith J.},
abstractNote = {Here, perovskite oxides are attractive candidates as catalysts for the electrolysis of water in alkaline energy storage and conversion systems. However, the rational design of active catalysts has been hampered by the lack of understanding of the mechanism of water electrolysis on perovskite surfaces. Key parameters that have been overlooked include the role of oxygen vacancies, B–O bond covalency, and redox activity of lattice oxygen species. Here we present a series of cobaltite perovskites where the covalency of the Co–O bond and the concentration of oxygen vacancies are controlled through Sr2+ substitution into La1–xSrxCoO3–δ. We attempt to rationalize the high activities of La1–xSrxCoO3–δ through the electronic structure and participation of lattice oxygen in the mechanism of water electrolysis as revealed through ab initio modelling. Using this approach, we report a material, SrCoO2.7, with a high, room temperature-specific activity and mass activity towards alkaline water electrolysis.},
doi = {10.1038/ncomms11053},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {2016},
month = {3}
}

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    A review of transition metal‐based bifunctional oxygen electrocatalysts
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    • Ibrahim, Kassa B.; Tsai, Meng‐Che; Chala, Soressa A.
    • Journal of the Chinese Chemical Society, Vol. 66, Issue 8
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    Atomic-scale perturbation of oxygen octahedra via surface ion exchange in perovskite nickelates boosts water oxidation
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    Amorphous Cobalt Iron Borate Grown on Carbon Paper as a Precatalyst for Water Oxidation
    journal, July 2019


    A review of transition metal‐based bifunctional oxygen electrocatalysts
    journal, April 2019

    • Ibrahim, Kassa B.; Tsai, Meng‐Che; Chala, Soressa A.
    • Journal of the Chinese Chemical Society, Vol. 66, Issue 8
    • DOI: 10.1002/jccs.201900001

    Atomic-scale perturbation of oxygen octahedra via surface ion exchange in perovskite nickelates boosts water oxidation
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