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Title: Enhancing perovskite electrocatalysis through strain tuning of oxygen deficiency

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/jacs.6b03520· OSTI ID:1263885
 [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)

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.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Organization:
USDOE Office of Science (SC); USDOE Laboratory Directed Research and Development (LDRD) Program
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1263885
Journal Information:
Journal of the American Chemical Society, Vol. 138, Issue 23; ISSN 0002-7863
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 181 works
Citation information provided by
Web of Science

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Cited By (44)

Tuning Bifunctional Oxygen Electrocatalysts by Changing the A-Site Rare-Earth Element in Perovskite Nickelates journal August 2018
Hydrothermal shape controllable synthesis of La 0.5 Sr 0.5 MnO 3 crystals and facet effect on electron transfer of oxygen reduction journal January 2018
The role of oxygen vacancies in water oxidation for perovskite cobalt oxide electrocatalysts: are more better? journal January 2019
Hierarchical Co(OH)F Superstructure Built by Low-Dimensional Substructures for Electrocatalytic Water Oxidation journal June 2017
Fabrication of a Mo‐Doped Strontium Cobaltite Perovskite Hybrid Supercapacitor Cell with High Energy Density and Excellent Cycling Life journal November 2018
Metal Oxide Nanocomposites: A Perspective from Strain, Defect, and Interface journal October 2018
Enhancing Electrocatalytic Water Splitting by Strain Engineering journal February 2019
Correlation between Ru–O hybridization and the oxygen evolution reaction in ruthenate epitaxial thin films journal January 2019
Cr‐Dopant Induced Breaking of Scaling Relations in CoFe Layered Double Hydroxides for Improvement of Oxygen Evolution Reaction journal July 2019
Regulating p-block metals in perovskite nanodots for efficient electrocatalytic water oxidation journal October 2017
Tuning oxygen electrocatalysis via strain on LaNiO 3 (001) journal January 2019
Atomic-resolution in-situ cooling study of oxygen vacancy ordering in La 0.5 Sr 0.5 CoO 3−δ thin films journal June 2019
Controlling Oxygen Mobility in Ruddlesden–Popper Oxides journal March 2017
Activation of ultrathin SrTiO 3 with subsurface SrRuO 3 for the oxygen evolution reaction journal January 2018
Strain coupling of oxygen non-stoichiometry in perovskite thin films journal December 2017
H2O2 decomposition catalyzed by strontium cobaltites and their application in Rhodamine B degradation in aqueous medium journal March 2019
Enhanced Electrocatalytic Oxygen Evolution Activity by Tuning Both the Oxygen Vacancy and Orbital Occupancy of B‐Site Metal Cation in NdNiO 3 journal June 2019
Oxygen vacancies in strained SrTiO 3 thin films: Formation enthalpy and manipulation journal April 2017
Interfacial Lattice‐Strain‐Driven Generation of Oxygen Vacancies in an Aerobic‐Annealed TiO 2 (B) Electrode journal November 2019
Reducing Oxygen Evolution Reaction Overpotential in Cobalt‐Based Electrocatalysts via Optimizing the “Microparticles‐in‐Spider Web” Electrode Configurations journal January 2020
Reversible Control of Physical Properties via an Oxygen-Vacancy-Driven Topotactic Transition in Epitaxial La 0.7 Sr 0.3 MnO 3− δ Thin Films journal December 2018
Transition metal oxide-based oxygen reduction reaction electrocatalysts for energy conversion systems with aqueous electrolytes journal January 2018
Recent Advances in Oxygen Electrocatalysts Based on Perovskite Oxides journal August 2019
Perovskite/Carbon Composites: Applications in Oxygen Electrocatalysis journal February 2017
Quasi-single-crystalline CoO hexagrams with abundant defects for highly efficient electrocatalytic water oxidation journal January 2018
3D Synergistically Active Carbon Nanofibers for Improved Oxygen Evolution journal March 2017
Ruthenium Oxide Nanosheets for Enhanced Oxygen Evolution Catalysis in Acidic Medium journal February 2019
Assemblage of Perovskite LaNiO 3 Connected With In Situ Grown Nitrogen-Doped Carbon Nanotubes as High-Performance Electrocatalyst for Oxygen Evolution Reaction journal July 2018
Magnesium-regulated oxygen vacancies of nickel layered double hydroxides for electrocatalytic water oxidation journal January 2018
Boosting water oxidation on metal-free carbon nanotubes via directional interfacial charge-transfer induced by an adsorbed polyelectrolyte journal January 2018
Recent Advances in Novel Nanostructuring Methods of Perovskite Electrocatalysts for Energy-Related Applications journal May 2018
The stability number as a metric for electrocatalyst stability benchmarking journal June 2018
In Situ Optical Absorption Studies of Point Defect Kinetics and Thermodynamics in Oxide Thin Films journal June 2019
Strain control of oxygen kinetics in the Ruddlesden-Popper oxide La1.85Sr0.15CuO4 journal January 2018
Controlling the Oxygen Electrocatalysis on Perovskite and Layered Oxide Thin Films for Solid Oxide Fuel Cell Cathodes journal March 2019
Stringing MOF-derived nanocages: a strategy for the enhanced oxygen evolution reaction journal January 2019
Tunable pH-dependent oxygen evolution activity of strontium cobaltite thin films for electrochemical water splitting journal January 2019
Heterogeneous integration of single-crystalline complex-oxide membranes journal February 2020
Novel Perovskite Materials for Thermal Water Splitting at Moderate Temperature journal August 2019
Design strategies for developing non-precious metal based bi-functional catalysts for alkaline electrolyte based zinc–air batteries journal January 2019
Surface Engineering of Nanostructured Energy Materials journal July 2018
Dynamic Tuning of a Thin Film Electrocatalyst by Tensile Strain journal November 2019
Sauerstoffreduktionsreaktion und Sauerstoffentwicklungsreaktionsmechanismen Untersuchung der nicht-edlen bifunktionellen Elektrokatalysatoren in alkalischem Elektrolyt text January 2018
Strain engineering of epitaxial oxide heterostructures beyond substrate limitations preprint January 2019

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