Understanding structure-property relations of Na-ion conductors is imperative for designing next generation all-solid batteries. We report a facile microwave-assisted synthesis of alpha-Na3PS4, a Na-ion solid electrolyte for, in the P phase with rapid, microwave-assisted heating to investigate the effect of vacancy defects on Na-ion diffusion and chemical stability at the electrolyte/metal electrode interface. We report phase purity for Na3PS4, as confirmed with X-ray diffraction, prepared from microwave-assisted heating as well as conventional solid-state furnace growth and mechanical milling. Additionally, we employ in-situ synchrotron X-ray scattering, in-situ Raman spectroscopy, and differential scanning calorimetry to investigate the local structure evolution through phase transformation, Na-ion disorder, and reorientational motions of the (PS4)3- anion upon heating of alpha-Na3PS4 from 25 to 300, which captures the tetragonal-to-cubic (beta-Na3PS4) phase transition at 257. Structural characterization information from X-ray scattering and Raman spectroscopy is cross-correlated with spatially-resolved transmission electron microscopy and selected area electron diffraction to investigate the interdiffusion and chemical decomposition of the solid electrolyte into binary PxSy and Na-(P,S) compounds at the metal electrode interface. The multi-modal characterization approach provides further insight into the effects of Na vacancy concentration on electrochemical performance and chemical stability of pristine Na3PS4 solid electrolyte as well as the solid electrolyte/Na interface.

Accelerated synthesis and local structure characterization of Na-ion solid electrolytes

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.