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

Abstract

Abstract 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 2.895 W 0.3 Sb 0.7 S 4 and Na 2.7 W 0.3 Sb 0.7 S 4 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 2.895 W 0.3 Sb 0.7 S 4 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. 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 2.895 W 0.3 Sb 0.7 S 4 as the primary SSE and a sodium sulfide (Na 2 S) cathode achieves a reversible capacity of 400 mAh g −1 .

Authors:
 [1]; ORCiD logo [2];  [1];  [1]; ORCiD logo [3];  [4];  [5];  [4]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]
  1. Univ. of Texas, Austin, TX (United States)
  2. Virginia Commonwealth Univ., Richmond, VA (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Argonne National Lab. (ANL), Lemont, IL (United States)
  5. Florida State Univ., Tallahassee, FL (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE
OSTI Identifier:
1856705
Alternate Identifier(s):
OSTI ID: 1829533
Grant/Contract Number:  
AC05-00OR22725; FG02-96ER45579; EE0008865; AC02-05CH11231; AC05 00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 60; Journal Issue: 50; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Na3SbS4; superionic conductor; sodium - sulfur battery; Solid-State Battery (SSB); sodium metal battery (SMB)

Citation Formats

Feng, Xuyong, Fang, Hong, Liu, Pengcheng, Wu, Nan, Self, Ethan C., Yin, Liang, Wang, Pengbo, Li, Xiang, Jena, Puru, Nanda, Jagjit, and Mitlin, David. Heavily Tungsten-Doped Sodium Thioantimonate Solid-State Electrolytes with Exceptionally Low Activation Energy for Ionic Diffusion. United States: N. p., 2021. Web. doi:10.1002/anie.202110699.
Feng, Xuyong, Fang, Hong, Liu, Pengcheng, Wu, Nan, Self, Ethan C., Yin, Liang, Wang, Pengbo, Li, Xiang, Jena, Puru, Nanda, Jagjit, & Mitlin, David. Heavily Tungsten-Doped Sodium Thioantimonate Solid-State Electrolytes with Exceptionally Low Activation Energy for Ionic Diffusion. United States. https://doi.org/10.1002/anie.202110699
Feng, Xuyong, Fang, Hong, Liu, Pengcheng, Wu, Nan, Self, Ethan C., Yin, Liang, Wang, Pengbo, Li, Xiang, Jena, Puru, Nanda, Jagjit, and Mitlin, David. Sun . "Heavily Tungsten-Doped Sodium Thioantimonate Solid-State Electrolytes with Exceptionally Low Activation Energy for Ionic Diffusion". United States. https://doi.org/10.1002/anie.202110699. https://www.osti.gov/servlets/purl/1856705.
@article{osti_1856705,
title = {Heavily Tungsten-Doped Sodium Thioantimonate Solid-State Electrolytes with Exceptionally Low Activation Energy for Ionic Diffusion},
author = {Feng, Xuyong and Fang, Hong and Liu, Pengcheng and Wu, Nan and Self, Ethan C. and Yin, Liang and Wang, Pengbo and Li, Xiang and Jena, Puru and Nanda, Jagjit and Mitlin, David},
abstractNote = {Abstract 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 2.895 W 0.3 Sb 0.7 S 4 and Na 2.7 W 0.3 Sb 0.7 S 4 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 2.895 W 0.3 Sb 0.7 S 4 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. 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 2.895 W 0.3 Sb 0.7 S 4 as the primary SSE and a sodium sulfide (Na 2 S) cathode achieves a reversible capacity of 400 mAh g −1 .},
doi = {10.1002/anie.202110699},
journal = {Angewandte Chemie (International Edition)},
number = 50,
volume = 60,
place = {United States},
year = {Sun Sep 26 00:00:00 EDT 2021},
month = {Sun Sep 26 00:00:00 EDT 2021}
}

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