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

Sahu, Gayatri; Rangasamy, Ezhiylmurugan; Li, Juchuan; Chen, Yan; An, Ke; Dudney, Nancy; Liang, Chengdu

doi:10.1039/c4ta01243g

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

Journal Article · Wed Apr 16 00:00:00 EDT 2014 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/c4ta01243g· OSTI ID:1154815

Sahu, Gayatri ^[1]; Rangasamy, Ezhiylmurugan ^[1]; Li, Juchuan ^[2]; Chen, Yan ^[3]; An, Ke ^[3]; Dudney, Nancy ^[2]; Liang, Chengdu ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Sources

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 Li_3.334Ge_0.334As_0.666S₄ 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.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC)

DOE Contract Number:: AC05-00OR22725

OSTI ID:: 1154815

Journal Information:: Journal of Materials Chemistry. A, Vol. 2, Issue 27; ISSN 2050-7488

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

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solid electrolyte
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