Designing Optimal Perovskite Structure for High Ionic Conduction
Abstract
Solid-oxide fuel/electrolyzer cells are limited by a dearth of electrolyte materials with low ohmic loss and an incomplete understanding of the structure-property relationships that would enable the rational design of better materials. In this work, using epitaxial thin-film growth, synchrotron radiation, impedance spectroscopy, and density-functional theory, the impact of structural parameters (i.e., unit-cell volume and octahedral rotations) on ionic conductivity is delineated in La0.9Sr0.1Ga0.95Mg0.05O3-σ. As compared to the zero-strain state, compressive strain reduces the unit-cell volume while maintaining large octahedral rotations, resulting in a strong reduction of ionic conductivity, while tensile strain increases the unit-cell volume while quenching octahedral rotations, resulting in a negligible effect on the ionic conductivity. Calculations reveal that larger unit-cell volumes and octahedral rotations decrease migration barriers and create low-energy migration pathways, respectively. The desired combination of large unit-cell volume and octahedral rotations is normally contraindicated, but through the creation of superlattice structures both expanded unit-cell volume and large octahedral rotations are experimentally realized, which result in an enhancement of the ionic conductivity. All told, the potential to tune ionic conductivity with structure alone by a factor of ≈ 2.5 at around 600 degrees C is observed, which sheds new light on the rational design ofmore »
- Authors:
-
[1];
- Univ. of California, Berkeley, CA (United States)
- Univ. of Illinois at Urbana-Champaign, IL (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Science and Technology of China, Hefei, Anhui (China)
- Pennsylvania State Univ., State College, PA (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Kyushu Univ., Fukuoka (Japan)
- Imperial College, London (United Kingdom)
- Univ. of Illinois at Urbana-Champaign, IL (United States); Kyushu Univ., Fukuoka (Japan)
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
- OSTI Identifier:
- 1633253
- Alternate Identifier(s):
- OSTI ID: 1573069; OSTI ID: 1615622
- Grant/Contract Number:
- AC02-06CH11357; AC02-05CH11231; OISE-1545907; W911NF-14-1-0104; SC0012375; DMR-1608938; DMR-1708615; AC02‐06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Materials
- Additional Journal Information:
- Journal Volume: 32; Journal Issue: 1; Journal ID: ISSN 0935-9648
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; crystal symmetry; energy conversion; ionic conduction; octahedral rotation; perovskite oxides; strain
Citation Formats
Gao, Ran, Jain, Abhinav C. P., Pandya, Shishir, Dong, Yongqi, Yuan, Yakun, Zhou, Hua, Dedon, Liv R., Thoréton, Vincent, Saremi, Sahar, Xu, Ruijuan, Luo, Aileen, Chen, Ting, Gopalan, Venkatraman, Ertekin, Elif, Kilner, John, Ishihara, Tatsumi, Perry, Nicola H., Trinkle, Dallas R., and Martin, Lane W. Designing Optimal Perovskite Structure for High Ionic Conduction. United States: N. p., 2019.
Web. doi:10.1002/adma.201905178.
Gao, Ran, Jain, Abhinav C. P., Pandya, Shishir, Dong, Yongqi, Yuan, Yakun, Zhou, Hua, Dedon, Liv R., Thoréton, Vincent, Saremi, Sahar, Xu, Ruijuan, Luo, Aileen, Chen, Ting, Gopalan, Venkatraman, Ertekin, Elif, Kilner, John, Ishihara, Tatsumi, Perry, Nicola H., Trinkle, Dallas R., & Martin, Lane W. Designing Optimal Perovskite Structure for High Ionic Conduction. United States. https://doi.org/10.1002/adma.201905178
Gao, Ran, Jain, Abhinav C. P., Pandya, Shishir, Dong, Yongqi, Yuan, Yakun, Zhou, Hua, Dedon, Liv R., Thoréton, Vincent, Saremi, Sahar, Xu, Ruijuan, Luo, Aileen, Chen, Ting, Gopalan, Venkatraman, Ertekin, Elif, Kilner, John, Ishihara, Tatsumi, Perry, Nicola H., Trinkle, Dallas R., and Martin, Lane W. Mon .
"Designing Optimal Perovskite Structure for High Ionic Conduction". United States. https://doi.org/10.1002/adma.201905178. https://www.osti.gov/servlets/purl/1633253.
@article{osti_1633253,
title = {Designing Optimal Perovskite Structure for High Ionic Conduction},
author = {Gao, Ran and Jain, Abhinav C. P. and Pandya, Shishir and Dong, Yongqi and Yuan, Yakun and Zhou, Hua and Dedon, Liv R. and Thoréton, Vincent and Saremi, Sahar and Xu, Ruijuan and Luo, Aileen and Chen, Ting and Gopalan, Venkatraman and Ertekin, Elif and Kilner, John and Ishihara, Tatsumi and Perry, Nicola H. and Trinkle, Dallas R. and Martin, Lane W.},
abstractNote = {Solid-oxide fuel/electrolyzer cells are limited by a dearth of electrolyte materials with low ohmic loss and an incomplete understanding of the structure-property relationships that would enable the rational design of better materials. In this work, using epitaxial thin-film growth, synchrotron radiation, impedance spectroscopy, and density-functional theory, the impact of structural parameters (i.e., unit-cell volume and octahedral rotations) on ionic conductivity is delineated in La0.9Sr0.1Ga0.95Mg0.05O3-σ. As compared to the zero-strain state, compressive strain reduces the unit-cell volume while maintaining large octahedral rotations, resulting in a strong reduction of ionic conductivity, while tensile strain increases the unit-cell volume while quenching octahedral rotations, resulting in a negligible effect on the ionic conductivity. Calculations reveal that larger unit-cell volumes and octahedral rotations decrease migration barriers and create low-energy migration pathways, respectively. The desired combination of large unit-cell volume and octahedral rotations is normally contraindicated, but through the creation of superlattice structures both expanded unit-cell volume and large octahedral rotations are experimentally realized, which result in an enhancement of the ionic conductivity. All told, the potential to tune ionic conductivity with structure alone by a factor of ≈ 2.5 at around 600 degrees C is observed, which sheds new light on the rational design of ion-conducting perovskite electrolytes.},
doi = {10.1002/adma.201905178},
journal = {Advanced Materials},
number = 1,
volume = 32,
place = {United States},
year = {Mon Nov 04 00:00:00 EST 2019},
month = {Mon Nov 04 00:00:00 EST 2019}
}
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