Influence of strain on SrFeO3-δ oxidation, reduction, and water dissociation: Insights from ambient pressure X-ray photoelectron spectroscopy
Abstract
The oxidation and reduction of metal oxides and their interaction with the environment play a critical role in their use for energy storage and conversion applications. The formation of surface adsorbates and their impact on oxide electronic structure can be challenging to probe experimentally, particularly for thin films which enable the study of epitaxial strain but have low surface areas. Here we present a detailed study using ambient pressure X-ray photoelectron spectroscopy of the reduction and oxidation of strained SrFeO3-δ, induced by changes in temperature, oxygen partial pressure, and water vapor exposure. We find that in comparison to the oxidized lattice, application of tensile strain promotes the formation of oxygen vacancies at the surface, facilitating the subsequent incorporation of oxygen into the lattice in an oxygen environment. While tensile strain does promote the formation of hydroxyls from water dissociation, the kinetics of this process appear more sluggish than on less-strained surfaces, likely due to a competitive surface interaction with oxygen or bulk absorption of hydroxyl species. These findings relating strain, oxygen vacancies, and surface reactivity yield important insight into the surface functionality of oxides for energy conversion and storage applications.
- Authors:
-
[1];
[1]
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Univ. of Science and Technology of China, Hefei (China)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- Publication Date:
- Research Org.:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1642419
- Alternate Identifier(s):
- OSTI ID: 1691766
- Report Number(s):
- PNNL-SA-152444
Journal ID: ISSN 0169-4332
- Grant/Contract Number:
- AC05-76RL01830; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Applied Surface Science
- Additional Journal Information:
- Journal Volume: 527; Journal ID: ISSN 0169-4332
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; ambient pressure X-ray photoelectron spectroscopy, perovskite, brownmillerite, strontium ferrite, hydroxylation, strain
Citation Formats
Stoerzinger, Kelsey A., Wang, Le, Su, Hongyang, Lee, Kyung-Jae, Crumlin, Ethan J., and Du, Yingge. Influence of strain on SrFeO3-δ oxidation, reduction, and water dissociation: Insights from ambient pressure X-ray photoelectron spectroscopy. United States: N. p., 2020.
Web. doi:10.1016/j.apsusc.2020.146919.
Stoerzinger, Kelsey A., Wang, Le, Su, Hongyang, Lee, Kyung-Jae, Crumlin, Ethan J., & Du, Yingge. Influence of strain on SrFeO3-δ oxidation, reduction, and water dissociation: Insights from ambient pressure X-ray photoelectron spectroscopy. United States. https://doi.org/10.1016/j.apsusc.2020.146919
Stoerzinger, Kelsey A., Wang, Le, Su, Hongyang, Lee, Kyung-Jae, Crumlin, Ethan J., and Du, Yingge. Mon .
"Influence of strain on SrFeO3-δ oxidation, reduction, and water dissociation: Insights from ambient pressure X-ray photoelectron spectroscopy". United States. https://doi.org/10.1016/j.apsusc.2020.146919. https://www.osti.gov/servlets/purl/1642419.
@article{osti_1642419,
title = {Influence of strain on SrFeO3-δ oxidation, reduction, and water dissociation: Insights from ambient pressure X-ray photoelectron spectroscopy},
author = {Stoerzinger, Kelsey A. and Wang, Le and Su, Hongyang and Lee, Kyung-Jae and Crumlin, Ethan J. and Du, Yingge},
abstractNote = {The oxidation and reduction of metal oxides and their interaction with the environment play a critical role in their use for energy storage and conversion applications. The formation of surface adsorbates and their impact on oxide electronic structure can be challenging to probe experimentally, particularly for thin films which enable the study of epitaxial strain but have low surface areas. Here we present a detailed study using ambient pressure X-ray photoelectron spectroscopy of the reduction and oxidation of strained SrFeO3-δ, induced by changes in temperature, oxygen partial pressure, and water vapor exposure. We find that in comparison to the oxidized lattice, application of tensile strain promotes the formation of oxygen vacancies at the surface, facilitating the subsequent incorporation of oxygen into the lattice in an oxygen environment. While tensile strain does promote the formation of hydroxyls from water dissociation, the kinetics of this process appear more sluggish than on less-strained surfaces, likely due to a competitive surface interaction with oxygen or bulk absorption of hydroxyl species. These findings relating strain, oxygen vacancies, and surface reactivity yield important insight into the surface functionality of oxides for energy conversion and storage applications.},
doi = {10.1016/j.apsusc.2020.146919},
journal = {Applied Surface Science},
number = ,
volume = 527,
place = {United States},
year = {Mon Jun 08 00:00:00 EDT 2020},
month = {Mon Jun 08 00:00:00 EDT 2020}
}
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