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Fundamental investigations on the sodium-ion transport properties of mixed polyanion solid-state battery electrolytes

Deng, Z and Mishra, TP and Mahayoni, E and Ma, Q and Tieu, AJK and Guillon, O and Chotard, J-N and Seznec, V and Cheetham, AK and Masquelier, C and Gautam, GS and Canepa, P (2022) Fundamental investigations on the sodium-ion transport properties of mixed polyanion solid-state battery electrolytes. In: Nature Communications, 13 (1).

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Official URL: https://doi.org/10.1038/s41467-022-32190-7


Lithium and sodium (Na) mixed polyanion solid electrolytes for all-solid-state batteries display some of the highest ionic conductivities reported to date. However, the effect of polyanion mixing on the ion-transport properties is still not fully understood. Here, we focus on Na1+xZr2SixP3−xO12 (0 ≤ x ≤ 3) NASICON electrolyte to elucidate the role of polyanion mixing on the Na-ion transport properties. Although NASICON is a widely investigated system, transport properties derived from experiments or theory vary by orders of magnitude. We use more than 2000 distinct ab initio-based kinetic Monte Carlo simulations to map the compositional space of NASICON over various time ranges, spatial resolutions and temperatures. Via electrochemical impedance spectroscopy measurements on samples with different sodium content, we find that the highest ionic conductivity (i.e., about 0.165 S cm–1 at 473 K) is experimentally achieved in Na3.4Zr2Si2.4P0.6O12, in line with simulations (i.e., about 0.170 S cm–1 at 473 K). The theoretical studies indicate that doped NASICON compounds (especially those with a silicon content x ≥ 2.4) can improve the Na-ion mobility compared to undoped NASICON compositions.

Item Type: Journal Article
Publication: Nature Communications
Publisher: Nature Research
Additional Information: The copyright for this article belongs to the Authors.
Department/Centre: Division of Mechanical Sciences > Materials Engineering (formerly Metallurgy)
Date Deposited: 22 Aug 2022 09:46
Last Modified: 22 Aug 2022 09:46
URI: https://eprints.iisc.ac.in/id/eprint/76140

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