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Under Pressure: Mechanochemical Effects on Structure and Ion Conduction in the Sodium-Ion Solid Electrolyte Na3PS4
- Source :
- Journal of the American Chemical Society, Journal of the American Chemical Society, 2020, 142 (43), pp.18422-18436. ⟨10.1021/jacs.0c06668⟩, Famprikis, T, Kudu, O U, Dawson, J A, Canepa, P, Fauth, F, Suard, E, Zbiri, M, Dambournet, D, Borkiewicz, O J, Bouyanfif, H, Emge, S P, Cretu, S, Chotard, J N, Grey, C P, Zeier, W G, Islam, M S & Masquelier, C 2020, ' Under pressure : Mechanochemical effects on structure and ion conduction in the sodium-ion solid electrolyte Na 3 PS 4 ', Journal of the American Chemical Society, vol. 142, no. 43, pp. 18422-18436 . https://doi.org/10.1021/jacs.0c06668
- Publication Year :
- 2020
- Publisher :
- American Chemical Society (ACS), 2020.
-
Abstract
- Fast-ion conductors are critical to the development of solid-state batteries. The effects of mechanochemical synthesis that lead to increased ionic conductivity in an archetypical sodium-ion conductor Na3PS4 are not fully understood. We present here a comprehensive analysis based on diffraction (Bragg, pair distribution function), spectroscopy (impedance, Raman, NMR, INS) and ab-initio simulations aimed at elucidating the synthesis-property relationships in Na3PS4. We consolidate previously reported interpretations about the local structure of ball-milled samples, underlining the sodium disorder and showing that a local tetragonal framework more accurately describes the structure than the originally proposed cubic one. Through variable-pressure impedance spectroscopy measurements, we report for the first time the activation volume for Na+ migration in Na3PS4, which is ~30% higher for the ball-milled samples. Moreover, we show that the effect of ball-milling on increasing the ionic conductivity of Na3PS4 to ~10-4 S/cm can be reproduced by applying external pressure on a sample from conventional high temperature ceramic synthesis. We conclude that the key effects of mechanochemical synthesis on the properties of solid electrolytes can be analyzed and understood in terms of pressure, strain and activation volume.
- Subjects :
- Materials science
Chemistry(all)
Ab initio
Thermodynamics
Electrolyte
010402 general chemistry
01 natural sciences
Biochemistry
Catalysis
Ion
Tetragonal crystal system
symbols.namesake
Colloid and Surface Chemistry
Fast ion conductor
Ionic conductivity
Ceramic
Chemistry
Pair distribution function
[CHIM.MATE]Chemical Sciences/Material chemistry
General Chemistry
0104 chemical sciences
Dielectric spectroscopy
visual_art
visual_art.visual_art_medium
symbols
Raman spectroscopy
Subjects
Details
- ISSN :
- 15205126 and 00027863
- Volume :
- 142
- Database :
- OpenAIRE
- Journal :
- Journal of the American Chemical Society
- Accession number :
- edsair.doi.dedup.....6596d6521dff72aa9214b7cdab85fd69