Under Pressure: Mechanochemical Effects on Structure and Ion Conduction in the Sodium-Ion Solid Electrolyte Na3PS4 - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue Journal of the American Chemical Society Année : 2020

Under Pressure: Mechanochemical Effects on Structure and Ion Conduction in the Sodium-Ion Solid Electrolyte Na3PS4

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Theodosios Famprikis
O. Ulas Kudu
  • Fonction : Auteur
  • PersonId : 1218565
  • IdRef : 257573003
James A. Dawson
  • Fonction : Auteur
Emmanuelle Suard
Steffen P. Emge
  • Fonction : Auteur

Résumé

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 and pair distribution function), spectroscopy (impedance, Raman, NMR and INS), and ab initio simulations aimed at elucidating the synthesis-property relationships in Na3PS4. We consolidate previously reported interpretations regarding 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 similar to 30% higher for the ball-milled samples. Moreover, we show that the effect of ball-milling on increasing the ionic conductivity of Na(3)PS(4 )to similar 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.

Domaines

Chimie Matériaux

Dates et versions

hal-03611087 , version 1 (16-03-2022)

Identifiants

Citer

Clare P. Grey, Wolfgang G. Zeier, M. Saiful Islam, Christian Masquelier, Theodosios Famprikis, et al.. Under Pressure: Mechanochemical Effects on Structure and Ion Conduction in the Sodium-Ion Solid Electrolyte Na3PS4. Journal of the American Chemical Society, 2020, 142 (43), pp.18422-18436. ⟨10.1021/jacs.0c06668⟩. ⟨hal-03611087⟩
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