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

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

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

Journal Article · Sun Jan 02 23:00:00 EST 2022 · Nature Energy

DOI:https://doi.org/10.1038/s41560-021-00952-0· OSTI ID:1869086

^[1]; ^[2]; ^[3]; Kim, Se Young ^[3]; Assoud, Abdeljalil ^[3]; ^[4]; ^[2]; ^[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)
Justus Liebig Univ., Giessen (Germany)
Univ. of Waterloo, ON (Canada). Waterloo Inst. for Nanotechnology
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

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. Additionally, high cathode loadings are also demonstrated in ASSBs with stable capacity retention of >4 mAh cm^-2 (~190 mAh g^-1).

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1869086

Journal Information:: Nature Energy, Journal Name: Nature Energy Journal Issue: 1 Vol. 7; ISSN 2058-7546

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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