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Title: An electrochemically stable homogeneous glassy electrolyte formed at room temperature for all-solid-state sodium batteries

Abstract

All-solid-state sodium batteries (ASSSBs) are promising candidates for grid-scale energy storage. However, there are no commercialized ASSSBs yet, in part due to the lack of a low-cost, simple-to-fabricate solid electrolyte (SE) with electrochemical stability towards Na metal. In this work, we report a family of oxysulfide glass SEs (Na3PS4-xOx, where 0 < x ≤ 60) that not only exhibit the highest critical current density among all Na-ion conducting sulfide-based SEs, but also enable high-performance ambient-temperature sodium-sulfur batteries. By forming bridging oxygen units, the Na3PS4-xOx SEs undergo pressure-induced sintering at room temperature, resulting in a fully homogeneous glass structure with robust mechanical properties. Furthermore, the self-passivating solid electrolyte interphase at the Na|SE interface is critical for interface stabilization and reversible Na plating and stripping. The new structural and compositional design strategies presented here provide a new paradigm in the development of safe, low-cost, energy-dense, and long-lifetime ASSSBs.

Authors:
 [1];  [2];  [2];  [3]; ORCiD logo [2];  [4]; ORCiD logo [4];  [5];  [5];  [6]; ORCiD logo [2];  [2]; ORCiD logo [5];  [7]; ORCiD logo [3]; ORCiD logo [2]
  1. Univ. of Houston, TX (United States); Chinese Academy of Sciences (CAS), Shanghai (China)
  2. Univ. of Houston, TX (United States)
  3. Iowa State Univ., Ames, IA (United States)
  4. Purdue Univ., West Lafayette, IN (United States)
  5. Rice Univ., Houston, TX (United States)
  6. Northern Illinois Univ., DeKalb, IL (United States)
  7. Univ. of California, Irvine, CA (United States)
Publication Date:
Research Org.:
Univ. of Houston, TX (United States)
Sponsoring Org.:
USDOE Advanced Research Projects Agency - Energy (ARPA-E); National Natural Science Foundation of China (NSFC)
OSTI Identifier:
1869512
Grant/Contract Number:  
AR0000654; 51901240
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 13; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Chi, Xiaowei, Zhang, Ye, Hao, Fang, Kmiec, Steven, Dong, Hui, Xu, Rong, Zhao, Kejie, Ai, Qing, Terlier, Tanguy, Wang, Liang, Zhao, Lihong, Guo, Liqun, Lou, Jun, Xin, Huolin L., Martin, Steve W., and Yao, Yan. An electrochemically stable homogeneous glassy electrolyte formed at room temperature for all-solid-state sodium batteries. United States: N. p., 2022. Web. doi:10.1038/s41467-022-30517-y.
Chi, Xiaowei, Zhang, Ye, Hao, Fang, Kmiec, Steven, Dong, Hui, Xu, Rong, Zhao, Kejie, Ai, Qing, Terlier, Tanguy, Wang, Liang, Zhao, Lihong, Guo, Liqun, Lou, Jun, Xin, Huolin L., Martin, Steve W., & Yao, Yan. An electrochemically stable homogeneous glassy electrolyte formed at room temperature for all-solid-state sodium batteries. United States. https://doi.org/10.1038/s41467-022-30517-y
Chi, Xiaowei, Zhang, Ye, Hao, Fang, Kmiec, Steven, Dong, Hui, Xu, Rong, Zhao, Kejie, Ai, Qing, Terlier, Tanguy, Wang, Liang, Zhao, Lihong, Guo, Liqun, Lou, Jun, Xin, Huolin L., Martin, Steve W., and Yao, Yan. Mon . "An electrochemically stable homogeneous glassy electrolyte formed at room temperature for all-solid-state sodium batteries". United States. https://doi.org/10.1038/s41467-022-30517-y. https://www.osti.gov/servlets/purl/1869512.
@article{osti_1869512,
title = {An electrochemically stable homogeneous glassy electrolyte formed at room temperature for all-solid-state sodium batteries},
author = {Chi, Xiaowei and Zhang, Ye and Hao, Fang and Kmiec, Steven and Dong, Hui and Xu, Rong and Zhao, Kejie and Ai, Qing and Terlier, Tanguy and Wang, Liang and Zhao, Lihong and Guo, Liqun and Lou, Jun and Xin, Huolin L. and Martin, Steve W. and Yao, Yan},
abstractNote = {All-solid-state sodium batteries (ASSSBs) are promising candidates for grid-scale energy storage. However, there are no commercialized ASSSBs yet, in part due to the lack of a low-cost, simple-to-fabricate solid electrolyte (SE) with electrochemical stability towards Na metal. In this work, we report a family of oxysulfide glass SEs (Na3PS4-xOx, where 0 < x ≤ 60) that not only exhibit the highest critical current density among all Na-ion conducting sulfide-based SEs, but also enable high-performance ambient-temperature sodium-sulfur batteries. By forming bridging oxygen units, the Na3PS4-xOx SEs undergo pressure-induced sintering at room temperature, resulting in a fully homogeneous glass structure with robust mechanical properties. Furthermore, the self-passivating solid electrolyte interphase at the Na|SE interface is critical for interface stabilization and reversible Na plating and stripping. The new structural and compositional design strategies presented here provide a new paradigm in the development of safe, low-cost, energy-dense, and long-lifetime ASSSBs.},
doi = {10.1038/s41467-022-30517-y},
journal = {Nature Communications},
number = 1,
volume = 13,
place = {United States},
year = {Mon May 23 00:00:00 EDT 2022},
month = {Mon May 23 00:00:00 EDT 2022}
}

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