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Title: Enhancing perovskite electrocatalysis through strain tuning of oxygen deficiency

Abstract

Oxygen vacancies in transition-metal oxides facilitate catalysis critical for energy storage and generation. However, promoting vacancies at the lower temperatures required for operation in devices such as metal–air batteries and portable fuel cells has proven elusive. Here we used thin films of perovskite-based strontium cobaltite (SrCoOx) to show that epitaxial strain is a powerful tool for manipulating the oxygen content under conditions consistent with the oxygen evolution reaction, yielding increasingly oxygen-deficient states in an environment where the cobaltite would normally be fully oxidized. The additional oxygen vacancies created through tensile strain enhance the cobaltite’s catalytic activity toward this important reaction by over an order of magnitude, equaling that of precious-metal catalysts, including IrO2. Lastly, our findings demonstrate that strain in these oxides can dictate the oxygen stoichiometry independent of ambient conditions, allowing unprecedented control over oxygen vacancies essential in catalysis near room temperature.

Authors:
 [1];  [2];  [2];  [2];  [2]
  1. National Institute of Standards and Technology, Gaithersburg, MD (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org.:
USDOE Office of Science (SC); USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1263885
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 138; Journal Issue: 23; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 30 DIRECT ENERGY CONVERSION

Citation Formats

Barron, Sara C., Lee, Ho Nyung, Petrie, Jonathan R., Jeen, Hyoungjeen, and Meyer, Tricia L. Enhancing perovskite electrocatalysis through strain tuning of oxygen deficiency. United States: N. p., 2016. Web. doi:10.1021/jacs.6b03520.
Barron, Sara C., Lee, Ho Nyung, Petrie, Jonathan R., Jeen, Hyoungjeen, & Meyer, Tricia L. Enhancing perovskite electrocatalysis through strain tuning of oxygen deficiency. United States. doi:10.1021/jacs.6b03520.
Barron, Sara C., Lee, Ho Nyung, Petrie, Jonathan R., Jeen, Hyoungjeen, and Meyer, Tricia L. Fri . "Enhancing perovskite electrocatalysis through strain tuning of oxygen deficiency". United States. doi:10.1021/jacs.6b03520. https://www.osti.gov/servlets/purl/1263885.
@article{osti_1263885,
title = {Enhancing perovskite electrocatalysis through strain tuning of oxygen deficiency},
author = {Barron, Sara C. and Lee, Ho Nyung and Petrie, Jonathan R. and Jeen, Hyoungjeen and Meyer, Tricia L.},
abstractNote = {Oxygen vacancies in transition-metal oxides facilitate catalysis critical for energy storage and generation. However, promoting vacancies at the lower temperatures required for operation in devices such as metal–air batteries and portable fuel cells has proven elusive. Here we used thin films of perovskite-based strontium cobaltite (SrCoOx) to show that epitaxial strain is a powerful tool for manipulating the oxygen content under conditions consistent with the oxygen evolution reaction, yielding increasingly oxygen-deficient states in an environment where the cobaltite would normally be fully oxidized. The additional oxygen vacancies created through tensile strain enhance the cobaltite’s catalytic activity toward this important reaction by over an order of magnitude, equaling that of precious-metal catalysts, including IrO2. Lastly, our findings demonstrate that strain in these oxides can dictate the oxygen stoichiometry independent of ambient conditions, allowing unprecedented control over oxygen vacancies essential in catalysis near room temperature.},
doi = {10.1021/jacs.6b03520},
journal = {Journal of the American Chemical Society},
number = 23,
volume = 138,
place = {United States},
year = {2016},
month = {5}
}

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Works referencing / citing this record:

In Situ Optical Absorption Studies of Point Defect Kinetics and Thermodynamics in Oxide Thin Films
journal, June 2019

  • Buckner, Haley B.; Perry, Nicola H.
  • Advanced Materials Interfaces, Vol. 6, Issue 15
  • DOI: 10.1002/admi.201900496

Design strategies for developing non-precious metal based bi-functional catalysts for alkaline electrolyte based zinc–air batteries
journal, January 2019

  • Han, Chao; Li, Weijie; Liu, Hua-Kun
  • Materials Horizons, Vol. 6, Issue 9
  • DOI: 10.1039/c9mh00502a

In Situ Optical Absorption Studies of Point Defect Kinetics and Thermodynamics in Oxide Thin Films
journal, June 2019

  • Buckner, Haley B.; Perry, Nicola H.
  • Advanced Materials Interfaces, Vol. 6, Issue 15
  • DOI: 10.1002/admi.201900496

Design strategies for developing non-precious metal based bi-functional catalysts for alkaline electrolyte based zinc–air batteries
journal, January 2019

  • Han, Chao; Li, Weijie; Liu, Hua-Kun
  • Materials Horizons, Vol. 6, Issue 9
  • DOI: 10.1039/c9mh00502a