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Title: High areal capacity, long cycle life 4 V ceramic all-solid-state Li-ion batteries enabled by chloride solid electrolytes

Abstract

All-solid-state Li batteries (ASSBs) employing inorganic solid electrolytes offer improved safety and are exciting candidates for next-generation energy storage. Herein, we report a family of lithium mixed-metal chlorospinels, Li2InxSc0.666-xCl4 (0 ≤ x ≤ 0.666), with high ionic conductivity (up to 2.0 mS cm-1) owing to a highly disordered Li-ion distribution, and low electronic conductivity (4.7 × 10-10 S cm-1), which are implemented for high-performance ASSBs. Owing to the excellent interfacial stability of the SE against uncoated high-voltage cathode materials, ASSBs utilizing LiCoO2 or LiNi0.85Co0.1Mn0.05O2 exhibit superior rate capability and long-term cycling (up to 4.8 V versus Li+/Li) compared to state-of-the-art ASSBs. In particular, the ASSB with LiNi0.85Co0.1Mn0.05O2 exhibits a long life of >3,000 cycles with 80% capacity retention at room temperature. Additionally, high cathode loadings are also demonstrated in ASSBs with stable capacity retention of >4 mAh cm-2 (~190 mAh g-1).

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3];  [3];  [3]; ORCiD logo [4]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of Waterloo, ON (Canada). Waterloo Inst. for Nanotechnology; Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research (JCESR)
  2. Justus Liebig Univ., Giessen (Germany)
  3. Univ. of Waterloo, ON (Canada). Waterloo Inst. for Nanotechnology
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1869086
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Nature Energy
Additional Journal Information:
Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2058-7546
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; batteries; electronic properties and materials

Citation Formats

Zhou, Laidong, Zuo, Tong-Tong, Kwok, Chun Yuen, Kim, Se Young, Assoud, Abdeljalil, Zhang, Qiang, Janek, Jürgen, and Nazar, Linda F. High areal capacity, long cycle life 4 V ceramic all-solid-state Li-ion batteries enabled by chloride solid electrolytes. United States: N. p., 2022. Web. doi:10.1038/s41560-021-00952-0.
Zhou, Laidong, Zuo, Tong-Tong, Kwok, Chun Yuen, Kim, Se Young, Assoud, Abdeljalil, Zhang, Qiang, Janek, Jürgen, & Nazar, Linda F. High areal capacity, long cycle life 4 V ceramic all-solid-state Li-ion batteries enabled by chloride solid electrolytes. United States. https://doi.org/10.1038/s41560-021-00952-0
Zhou, Laidong, Zuo, Tong-Tong, Kwok, Chun Yuen, Kim, Se Young, Assoud, Abdeljalil, Zhang, Qiang, Janek, Jürgen, and Nazar, Linda F. Mon . "High areal capacity, long cycle life 4 V ceramic all-solid-state Li-ion batteries enabled by chloride solid electrolytes". United States. https://doi.org/10.1038/s41560-021-00952-0. https://www.osti.gov/servlets/purl/1869086.
@article{osti_1869086,
title = {High areal capacity, long cycle life 4 V ceramic all-solid-state Li-ion batteries enabled by chloride solid electrolytes},
author = {Zhou, Laidong and Zuo, Tong-Tong and Kwok, Chun Yuen and Kim, Se Young and Assoud, Abdeljalil and Zhang, Qiang and Janek, Jürgen and Nazar, Linda F.},
abstractNote = {All-solid-state Li batteries (ASSBs) employing inorganic solid electrolytes offer improved safety and are exciting candidates for next-generation energy storage. Herein, we report a family of lithium mixed-metal chlorospinels, Li2InxSc0.666-xCl4 (0 ≤ x ≤ 0.666), with high ionic conductivity (up to 2.0 mS cm-1) owing to a highly disordered Li-ion distribution, and low electronic conductivity (4.7 × 10-10 S cm-1), which are implemented for high-performance ASSBs. Owing to the excellent interfacial stability of the SE against uncoated high-voltage cathode materials, ASSBs utilizing LiCoO2 or LiNi0.85Co0.1Mn0.05O2 exhibit superior rate capability and long-term cycling (up to 4.8 V versus Li+/Li) compared to state-of-the-art ASSBs. In particular, the ASSB with LiNi0.85Co0.1Mn0.05O2 exhibits a long life of >3,000 cycles with 80% capacity retention at room temperature. Additionally, high cathode loadings are also demonstrated in ASSBs with stable capacity retention of >4 mAh cm-2 (~190 mAh g-1).},
doi = {10.1038/s41560-021-00952-0},
journal = {Nature Energy},
number = 1,
volume = 7,
place = {United States},
year = {Mon Jan 03 00:00:00 EST 2022},
month = {Mon Jan 03 00:00:00 EST 2022}
}

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