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Title: Nanoscale structural oscillations in perovskite oxides induced by oxygen evolution

Abstract

Understanding the interaction between water and oxides is critical for many technological applications, including energy storage, surface wetting/self-cleaning, photocatalysis and sensors. In this paper, we report observations of strong structural oscillations of Ba0.5Sr0.5Co0.8Fe0.2O3$-$δ (BSCF) in the presence of both H2O vapour and electron irradiation using environmental transmission electron microscopy. These oscillations are related to the formation and collapse of gaseous bubbles. Electron energy-loss spectroscopy provides direct evidence of O2 formation in these bubbles due to the incorporation of H2O into BSCF. SrCoO3$-$δ was found to exhibit small oscillations, while none were observed for La0.5Sr0.5CoO3$-$δ and LaCoO3. The structural oscillations of BSCF can be attributed to the fact that its oxygen 2p-band centre is close to the Fermi level, which leads to a low energy penalty for oxygen vacancy formation, high ion mobility, and high water uptake. This work provides surprising insights into the interaction between water and oxides under electron-beam irradiation.

Authors:
ORCiD logo [1];  [1];  [2];  [3]; ORCiD logo [3];  [4]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering
  2. Ecole Polytechnique Federale Lausanne (Switzlerland). Inst. of Materials
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  4. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering; Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Mechanical Engineering
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1349577
Report Number(s):
BNL-113716-2017-JA
Journal ID: ISSN 1476-1122; R&D Project: 16060; 16060; KC0403020; TRN: US1701581
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 16; Journal Issue: 1; Journal ID: ISSN 1476-1122
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 25 ENERGY STORAGE; water splitting; photocatalysis; electron beam interactions; Center for Functional Nanomaterials

Citation Formats

Han, Binghong, Stoerzinger, Kelsey A., Tileli, Vasiliki, Gamalski, Andrew  D., Stach, Eric A., and Shao-Horn, Yang. Nanoscale structural oscillations in perovskite oxides induced by oxygen evolution. United States: N. p., 2016. Web. doi:10.1038/nmat4764.
Han, Binghong, Stoerzinger, Kelsey A., Tileli, Vasiliki, Gamalski, Andrew  D., Stach, Eric A., & Shao-Horn, Yang. Nanoscale structural oscillations in perovskite oxides induced by oxygen evolution. United States. doi:10.1038/nmat4764.
Han, Binghong, Stoerzinger, Kelsey A., Tileli, Vasiliki, Gamalski, Andrew  D., Stach, Eric A., and Shao-Horn, Yang. Mon . "Nanoscale structural oscillations in perovskite oxides induced by oxygen evolution". United States. doi:10.1038/nmat4764. https://www.osti.gov/servlets/purl/1349577.
@article{osti_1349577,
title = {Nanoscale structural oscillations in perovskite oxides induced by oxygen evolution},
author = {Han, Binghong and Stoerzinger, Kelsey A. and Tileli, Vasiliki and Gamalski, Andrew  D. and Stach, Eric A. and Shao-Horn, Yang},
abstractNote = {Understanding the interaction between water and oxides is critical for many technological applications, including energy storage, surface wetting/self-cleaning, photocatalysis and sensors. In this paper, we report observations of strong structural oscillations of Ba0.5Sr0.5Co0.8Fe0.2O3$-$δ (BSCF) in the presence of both H2O vapour and electron irradiation using environmental transmission electron microscopy. These oscillations are related to the formation and collapse of gaseous bubbles. Electron energy-loss spectroscopy provides direct evidence of O2 formation in these bubbles due to the incorporation of H2O into BSCF. SrCoO3$-$δ was found to exhibit small oscillations, while none were observed for La0.5Sr0.5CoO3$-$δ and LaCoO3. The structural oscillations of BSCF can be attributed to the fact that its oxygen 2p-band centre is close to the Fermi level, which leads to a low energy penalty for oxygen vacancy formation, high ion mobility, and high water uptake. This work provides surprising insights into the interaction between water and oxides under electron-beam irradiation.},
doi = {10.1038/nmat4764},
journal = {Nature Materials},
number = 1,
volume = 16,
place = {United States},
year = {2016},
month = {10}
}

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