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F and N Rich Solid Electrolyte for Stable All-Solid-State Battery

Journal Article · · Advanced Functional Materials
We report the instability of sulfide solid electrolytes to Li anode and high-voltage LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes limits the cyclic performance of all-solid-state lithium battery (ASSLB). Herein, the stability of Li6PS5Cl against Li anode is enhanced by mixing a small amount (0.32 wt%) of CuF2-LiNO3 (CL) into Li6PS5Cl electrolyte layer to in-situ form a mixed-conductive-lithiophobic and self-healing LiF-Li3N-Cu solid electrolyte interphase (SEI) at Li6PS5Cl-CL/Li interface. The critical current density (CCD) of Li6PS5Cl-CuF2-LiNO3 increases to 1.4 mA cm–2/1.4 mAh cm–2 at room temperature, which is much higher than that of pristine Li6PS5Cl (0.4 mA cm–2/0.4 mAh cm–2) even though mixing 0.32 wt% CL into Li6PS5Cl slightly reduces the ionic conductivity from 2.9 × 10–3 to 1.5 × 10–3 S cm–1. The compatibility of Li6PS5Cl-CL electrolyte to single-crystalline NMC811 (S-NMC811) is further enhanced by adding a small amount (0.02 wt%) of AlF3 into Li6PS5Cl-CL forming Li6PS5Cl-CuF2-LiNO3-AlF3 (Li6>PS5Cl-CLA) as a cathode electrolyte and by doing Cl on S-NMC811 (Cl@S-NMC811) surface. The Cl@S-NMC811-Li6PS5Cl-CLA|Li6PS5Cl-CL|Li cells with areal capacity of 2.55 mAh cm-2 achieve a capacity retention of 69.4% after 100 cycles at 1C (1C = 200 mAh g-1). Adding a small amount of SEI and cathode/electrolyte interphase (CEI) former into the sulfide electrolytes with minimal reduction (48.3%) of ionic conductivity is an effective method to enhance the performance of ASSLB.
Research Organization:
University of California, San Diego, CA (United States); University of Maryland, College Park, MD (United States)
Sponsoring Organization:
USDOE Advanced Research Projects Agency - Energy (ARPA-E)
Grant/Contract Number:
AR0000781; EE0008856
OSTI ID:
1976185
Alternate ID(s):
OSTI ID: 1837707
OSTI ID: 23130458
Journal Information:
Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 15 Vol. 32; ISSN 1616-301X
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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