Journal
JOURNAL OF MATERIALS CHEMISTRY A
Volume 9, Issue 26, Pages 15012-15018Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1ta03042f
Keywords
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Funding
- U.S. Department of Energy's Office of Energy Efficiency and Renewable Energy (EERE) under the National Energy Technology Lab Award [DE-EE0008859]
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A thin argyrodite (Li6PS5Cl) protection layer was reported to prevent the unstable interaction between halide electrolytes and Li metal anodes. Experimental results demonstrated highly stable Li plating/stripping cycling and enhanced performance of solid-state batteries with this protective layer.
Despite their excellent ionic conductivity and electrochemical oxidative stability, the emerging halide-based solid electrolytes suffer from inherent instability toward Li metal anodes. A thick and resistive interface can be formed by continuous reaction between halide electrolytes and Li anodes, leading to high impedance, low coulombic efficiency, and even short circuit of solid-state cells. Here, we report a thin argyrodite (Li6PS5Cl) protection layer to avoid the direct physical contact of the Li anode with Li3YCl6, a representative halide electrolyte. Li6PS5Cl is kinetically stable towards lithium and can also form a good hetero-contact with Li3YCl6. Highly stable Li plating/stripping cycling of a symmetric cell with a steady overpotential of 100 mV after 1000 h was demonstrated, compared to severe overpotential build-up to reach 1500 mV after 60 h of the control group. Besides, the LiNi0.8Co0.1Mn0.1O2/Li full solid-state cell displayed a high initial coulombic efficiency of >87% and a stable lifetime of over 100 cycles. The facile protection of Li6PS5Cl provides a universal way to prevent unfavorable interaction at the anode interface and realize high performance all-solid-state Li-metal batteries.
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