Journal
ADVANCED MATERIALS
Volume 32, Issue 34, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202000223
Keywords
cryo-transmission electron microscopy; interfaces; lithium metal anodes; polymer electrolytes
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Funding
- National Natural Science Foundation of China [21902144, U1802254, 51972285, 51722210] Funding Source: Medline
- Natural Science Foundation of Zhejiang Province [LQ20E030012, LD18E020003, LY17E020010] Funding Source: Medline
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The application of solid polymer electrolytes (SPEs) is still inherently limited by the unstable lithium (Li)/electrolyte interface, despite the advantages of security, flexibility, and workability of SPEs. Herein, the Li/electrolyte interface is modified by introducing Li2S additive to harvest stable all-solid-state lithium metal batteries (LMBs). Cryo-transmission electron microscopy (cryo-TEM) results demonstrate a mosaic interface between poly(ethylene oxide) (PEO) electrolytes and Li metal anodes, in which abundant crystalline grains of Li, Li2O, LiOH, and Li(2)CO(3)are randomly distributed. Besides, cryo-TEM visualization, combined with molecular dynamics simulations, reveals that the introduction of Li2S accelerates the decomposition of N(CF3SO2)(2)(-)and consequently promotes the formation of abundant LiF nanocrystals in the Li/PEO interface. The generated LiF is further verified to inhibit the breakage of C-O bonds in the polymer chains and prevents the continuous interface reaction between Li and PEO. Therefore, the all-solid-state LMBs with the LiF-enriched interface exhibit improved cycling capability and stability in a cell configuration with an ultralong lifespan over 1800 h. This work is believed to open up a new avenue for rational design of high-performance all-solid-state LMBs.
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