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/ange.202110699

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

Journal Article · 08 November 2021 · Angewandte Chemie

DOI: https://doi.org/10.1002/ange.202110699 · OSTI ID:1829372

Feng, Xuyong ^[1];

^[2]; Liu, Pengcheng ^[1]; Wu, Nan ^[1]; Self, Ethan C. ^[3]; Yin, Liang ^[4]; Wang, Pengbo ^[5]; Li, Xiang ^[6];

^[2]; Nanda, Jagjit ^[3];

^[1]

Materials Science and Engineering Program &, Texas Materials Institute (TMI) The University of Texas at Austin Austin TX 78712-1591 USA
Department of Physics Virginia Commonwealth University Richmond VA 23284 USA
Chemical Sciences Division Oak Ridge National Laboratory Oak Ridge TN 37830 USA
X-ray Science Division Argonne National Laboratory 9700 South Cass Avenue Lemont IL 60439 USA
Department of Chemistry and Biochemistry Florida State University Tallahassee FL 32306 USA
Argonne National Laboratory 9700S. Cass Avenue Lemont IL 60439 USA

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 .

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Sponsoring Organization:: USDOE

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

OSTI ID:: 1829372

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Vol. 133 Journal Issue: 50; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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