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Title: A high-conduction Ge substituted Li3AsS4 solid electrolyte with exceptional low activation energy

In lithium-ion conducting solid electrolytes the potential to enable high-energy-density secondary batteries and offer distinctive safety features as an advantage over traditional liquid electrolytes is shown. Achieving the combination of high ionic conductivity, low activation energy, and outstanding electrochemical stability in crystalline solid electrolytes is a challenge for the synthesis of novel solid electrolytes. We report an exceptionally low activation energy (Ea) and high room temperature superionic conductivity via facile aliovalent substitution of Li3AsS4 by Ge, which increased the conductivity by two orders of magnitude as compared to the parent compound. The composition Li3.334Ge0.334As0.666S4 has a high ionic conductivity of 1.12 mScm-1 at 27°C. Local Li+ hopping in this material is accompanied by distinctive low activation energy Ea of 0.17 eV being the lowest of Li+ solid conductors. Finally, our study demonstrates the efficacy of surface passivation of solid electrolyte to achieve compatibility with metallic lithium electrodes.
Authors:
 [1] ;  [1] ;  [2] ;  [3] ;  [3] ;  [2] ;  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Sources
Publication Date:
OSTI Identifier:
1154815
DOE Contract Number:
AC05-00OR22725
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Materials Chemistry. A; Journal Volume: 2; Journal Issue: 27
Publisher:
Royal Society of Chemistry
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE solid electrolyte; lithium batteries; energy storage; lithium-sulfur batteries