On the origin of high ionic conductivity in Na-doped SrSiO3
Abstract
Understanding the local structure and ion dynamics is at the heart of ion conductor research. This paper reports on high-resolution solid-state 29Si, 23Na, and 17O NMR investigation of the structure, chemical composition, and ion dynamics of a newly discovered fast ion conductor, Na-doped SrSiO3, which exhibited a much higher ionic conductivity than most of current oxide ion conductors. Quantitative analyses reveal that with a small dose (<10 mol%) of Na, the doped Na integrates into the SrSiO3 structure to form NaxSr1-xSiO3-0.5x, and with >10 mol% Na doping, phase separation occurs, leading to the formation of an amorphous phase β-Na2Si2O5 and a crystalline Sr-rich phase. Variable-temperature 23Na and 17O magic-angle-spinning NMR up to 618 °C have shown significant changes in Na ion dynamics at high temperatures but little oxide ion motion, suggesting that Na ions are responsible for the observed high ionic conductivity. In addition, β-Na2Si2O5 starts to crystallize at temperatures higher than 480 °C with prolonged heating, resulting in reduction in Na+ motion, and thus degradation of ionic conductivity. This study has contributed critical evidence to the understanding of ionic conduction in Na-doped SrSiO3 and demonstrated that multinuclear high-resolution and high-temperature solid-state NMR is a uniquely useful tool for investigatingmore »
- Authors:
-
- Florida State Univ., Tallahassee, FL (United States). Dept. of Chemistry and Biochemistry
- Univ. of South Carolina, Columbia, SC (United States). Dept. of Mechanical Engineering
- Florida State Univ., Tallahassee, FL (United States). Dept. of Scientific Computing
- Radboud Univ., Nijmegen (Netherlands). Inst. for Molecules and Materials
- Florida State Univ., Tallahassee, FL (United States). National High Magnetic Field Lab. (MagLab). Centre of Interdisciplinary Magnetic Resonance
- Florida State Univ., Tallahassee, FL (United States). Dept. of Chemistry and Biochemistry; Florida State Univ., Tallahassee, FL (United States). National High Magnetic Field Lab. (MagLab). Centre of Interdisciplinary Magnetic Resonance
- Publication Date:
- Research Org.:
- Univ. of South Carolina, Columbia, SC (United States); Florida State Univ., Tallahassee, FL (United States)
- Sponsoring Org.:
- USDOE Advanced Research Projects Agency - Energy (ARPA-E); National Science Foundation (NSF)
- OSTI Identifier:
- 1437305
- Alternate Identifier(s):
- OSTI ID: 1418583
- Grant/Contract Number:
- AR0000492; 1508404
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemical Science
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 6; Journal ID: ISSN 2041-6520
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE
Citation Formats
Chien, Po-Hsiu, Jee, Youngseok, Huang, Chen, Dervi?o?lu, Riza, Hung, Ivan, Gan, Zhehong, Huang, Kevin, and Hu, Yan-Yan. On the origin of high ionic conductivity in Na-doped SrSiO3. United States: N. p., 2016.
Web. doi:10.1039/c5sc04270d.
Chien, Po-Hsiu, Jee, Youngseok, Huang, Chen, Dervi?o?lu, Riza, Hung, Ivan, Gan, Zhehong, Huang, Kevin, & Hu, Yan-Yan. On the origin of high ionic conductivity in Na-doped SrSiO3. United States. https://doi.org/10.1039/c5sc04270d
Chien, Po-Hsiu, Jee, Youngseok, Huang, Chen, Dervi?o?lu, Riza, Hung, Ivan, Gan, Zhehong, Huang, Kevin, and Hu, Yan-Yan. Wed .
"On the origin of high ionic conductivity in Na-doped SrSiO3". United States. https://doi.org/10.1039/c5sc04270d. https://www.osti.gov/servlets/purl/1437305.
@article{osti_1437305,
title = {On the origin of high ionic conductivity in Na-doped SrSiO3},
author = {Chien, Po-Hsiu and Jee, Youngseok and Huang, Chen and Dervi?o?lu, Riza and Hung, Ivan and Gan, Zhehong and Huang, Kevin and Hu, Yan-Yan},
abstractNote = {Understanding the local structure and ion dynamics is at the heart of ion conductor research. This paper reports on high-resolution solid-state 29Si, 23Na, and 17O NMR investigation of the structure, chemical composition, and ion dynamics of a newly discovered fast ion conductor, Na-doped SrSiO3, which exhibited a much higher ionic conductivity than most of current oxide ion conductors. Quantitative analyses reveal that with a small dose (<10 mol%) of Na, the doped Na integrates into the SrSiO3 structure to form NaxSr1-xSiO3-0.5x, and with >10 mol% Na doping, phase separation occurs, leading to the formation of an amorphous phase β-Na2Si2O5 and a crystalline Sr-rich phase. Variable-temperature 23Na and 17O magic-angle-spinning NMR up to 618 °C have shown significant changes in Na ion dynamics at high temperatures but little oxide ion motion, suggesting that Na ions are responsible for the observed high ionic conductivity. In addition, β-Na2Si2O5 starts to crystallize at temperatures higher than 480 °C with prolonged heating, resulting in reduction in Na+ motion, and thus degradation of ionic conductivity. This study has contributed critical evidence to the understanding of ionic conduction in Na-doped SrSiO3 and demonstrated that multinuclear high-resolution and high-temperature solid-state NMR is a uniquely useful tool for investigating ion conductors at their operating conditions.},
doi = {10.1039/c5sc04270d},
journal = {Chemical Science},
number = 6,
volume = 7,
place = {United States},
year = {Wed Feb 17 00:00:00 EST 2016},
month = {Wed Feb 17 00:00:00 EST 2016}
}
Web of Science
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