Heavily Tungsten-Doped Sodium Thioantimonate Solid-State Electrolytes with Exceptionally Low Activation Energy for Ionic Diffusion

Feng, Xuyong; Fang, Hong; Liu, Pengcheng; Wu, Nan; Self, Ethan C.; Yin, Liang; Wang, Pengbo; Li, Xiang; Jena, Puru; Nanda, Jagjit; Mitlin, David

doi:10.1002/anie.202110699

Heavily Tungsten-Doped Sodium Thioantimonate Solid-State Electrolytes with Exceptionally Low Activation Energy for Ionic Diffusion

Journal Article · Sun Sep 26 00:00:00 EDT 2021 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202110699· OSTI ID:1856705

Feng, Xuyong ^[1]; ^[2]; Liu, Pengcheng ^[1]; Wu, Nan ^[1]; ^[3]; Yin, Liang ^[4]; Wang, Pengbo ^[5]; Li, Xiang ^[4]; ^[2]; ^[3]; ^[1]

Univ. of Texas, Austin, TX (United States)
Virginia Commonwealth Univ., Richmond, VA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Florida State Univ., Tallahassee, FL (United States)

A strategy for modifying the structure of solid-state electrolytes (SSEs) to reduce the cation diffusion activation energy is presented. Two heavily W-doped sodium thioantimonate SSEs, Na_2.895W_0.3Sb_0.7S₄ and Na_2.7W_0.3Sb_0.7S₄ are designed, both exhibiting exceptionally low activation energy and enhanced room temperature (RT) ionic conductivity; 0.09 eV, 24.2 mS/cm and 0.12 eV, 14.5 mS/cm. At –15 °C the Na_2.895W_0.3Sb_0.7S₄ displays a total ionic conductivity of 5.5 mS/cm. The 30 % W content goes far beyond the 10–12 % reported in the prior studies, and results in novel pseudo-cubic or orthorhombic structures. Here, calculations reveal that these properties result from a combination of multiple diffusion mechanisms, including vacancy defects, strongly correlated modes and excessive Na-ions. An all-solid-state battery (ASSB) using Na_2.895W_0.3Sb_0.7S₄ as the primary SSE and a sodium sulfide (Na₂S) cathode achieves a reversible capacity of 400 mAh g^–1.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-05CH11231; AC05-00OR22725; EE0008865; FG02-96ER45579

OSTI ID:: 1856705

Alternate ID(s):: OSTI ID: 1829533
OSTI ID: 23096209

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 50 Vol. 60; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Heavily Tungsten–Doped Sodium Thioantimonate Solid–State Electrolytes with Exceptionally Low Activation Energy for Ionic Diffusion

Journal Article · Sat Sep 25 20:00:00 EDT 2021 · Angewandte Chemie · OSTI ID:2532488

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Heavily Tungsten-Doped Sodium Thioantimonate Solid-State Electrolytes with Exceptionally Low Activation Energy for Ionic Diffusion

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