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

Laidong Zhou; Tong Tong Zuo; Chun Yuen Kwok; Se Young Kim; Abdeljalil Assoud; Qiang Zhang; Jürgen Janek; Linda F. Nazar

doi:10.1038/s41560-021-00952-0

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

Laidong Zhou, Tong Tong Zuo, Chun Yuen Kwok, Se Young Kim, Abdeljalil Assoud, Qiang Zhang, Jürgen Janek, Linda F. Nazar

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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, Li₂In_xSc_0.666−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 LiNi_0.85Co_0.1Mn_0.05O₂ 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 LiNi_0.85Co_0.1Mn_0.05O₂ exhibits a long life of >3,000 cycles with 80% capacity retention at room temperature. High cathode loadings are also demonstrated in ASSBs with stable capacity retention of >4 mAh cm⁻² (~190 mAh g⁻¹).

Original language	English
Pages (from-to)	83-93
Number of pages	11
Journal	Nature Energy
Volume	7
Issue number	1
DOIs	https://doi.org/10.1038/s41560-021-00952-0
State	Published - Jan 2022

Funding

This work was supported by the Joint Center for Energy Storage Research, an Energy Innovation Hub funded by the US Department of Energy, Office of Science, Basic Energy Sciences and NSERC via their Canada Research Chair and Discovery Grant programmes. The neutron diffraction measurement at the POWGEN instrument at Oak Ridge National Laboratory, Spallation Neutron Source, was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy. TOF-SIMS measurements were performed at the Justus Liebig University Giessen (funding through Bundesministerium für Bildung und Forschung projects 03XP0177D/03XP0228C). We thank BASF SE for providing NCM622 and NCM85 cathode active materials.

Funders	Funder number
Joint Center for Energy Storage Research
Scientific User Facilities Division
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Oak Ridge National Laboratory
Government of Canada
Natural Sciences and Engineering Research Council of Canada

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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. High cathode loadings are also demonstrated in ASSBs with stable capacity retention of >4 mAh cm−2 (~190 mAh g−1).",

author = "Laidong Zhou and Zuo, {Tong Tong} and Kwok, {Chun Yuen} and Kim, {Se Young} and Abdeljalil Assoud and Qiang Zhang and J{\"u}rgen Janek and Nazar, {Linda F.}",

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AU - Assoud, Abdeljalil

AU - Zhang, Qiang

AU - Janek, Jürgen

AU - Nazar, Linda F.

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N2 - 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. High cathode loadings are also demonstrated in ASSBs with stable capacity retention of >4 mAh cm−2 (~190 mAh g−1).

AB - 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. High cathode loadings are also demonstrated in ASSBs with stable capacity retention of >4 mAh cm−2 (~190 mAh g−1).

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

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