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

• DOI: 10.1021/jacs.0c06668
• Publication Date: 2020-10-15T13:13:01Z
• Authors: Theodosios Famprikis; Ö. Ulaş Kudu; James A. Dawson; Pieremanuele Canepa; François Fauth; Emmanuelle Suard; Mohamed Zbiri; Damien Dambournet; Olaf J. Borkiewicz; Houssny Bouyanfif; Steffen P. Emge; Sorina Cretu; Jean-Noël Chotard; Clare P. Grey; Wolfgang G. Zeier; M. Saiful Islam; Christian Masquelier
• Keywords: Fast ion conductor

Fast-ion conductors are critical to the development of solid-state batteries. The effects mechanochemical synthesis that lead increased ionic conductivity in an archetypical sodium-ion conductor Na3PS4 not fully understood. We present here a comprehensive analysis based on diffraction (Bragg and pair distribution function), spectroscopy (impedance, Raman, NMR INS), ab initio simulations aimed at elucidating synthesis-property relationships Na3PS4. consolidate previously reported interpretations regarding local structure ball-milled samples, underlining sodium disorder showing tetragonal framework more accurately describes than originally proposed cubic one. Through variable-pressure impedance measurements, we report for first time activation volume Na+ migration Na3PS4, which is ∼30% higher samples. Moreover, show effect ball-milling increasing ∼10-4 S/cm can be reproduced by applying external pressure sample from conventional high-temperature ceramic synthesis. conclude key properties solid electrolytes analyzed understood terms pressure, strain, volume.