On the origin of high ionic conductivity in Na-doped SrSiO3

Chien, Po-Hsiu; Jee, Youngseok; Huang, Chen; Dervi?o?lu, Riza; Hung, Ivan; Gan, Zhehong; Huang, Kevin; Hu, Yan-Yan

doi:10.1039/c5sc04270d

Title: On the origin of high ionic conductivity in Na-doped SrSiO₃

Journal Article · Wed Feb 17 00:00:00 EST 2016 · Chemical Science

DOI:https://doi.org/10.1039/c5sc04270d· OSTI ID:1437305

^[1]; Jee, Youngseok ^[2]; Huang, Chen ^[3];

^[4]; Hung, Ivan ^[5]; Gan, Zhehong ^[5]; Huang, Kevin ^[2];

^[6]

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

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 Na_xSr_1-xSiO_3-0.5x, 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.

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Research Organization:: Univ. of South Carolina, Columbia, SC (United States); Florida State Univ., Tallahassee, FL (United States)

Sponsoring Organization:: USDOE Advanced Research Projects Agency - Energy (ARPA-E); National Science Foundation (NSF)

Grant/Contract Number:: AR0000492; 1508404

OSTI ID:: 1437305

Alternate ID(s):: OSTI ID: 1418583

Journal Information:: Chemical Science, Vol. 7, Issue 6; ISSN 2041-6520

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 17 works

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