4.8 Article

Immobilizing Ceramic Electrolyte Particles into a Gel Matrix Formed In Situ for Stable Li-Metal Batteries

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 32, Pages 38179-38187

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c05602

Keywords

hybrid solid / gel electrolytes; in situ gel; LLZO; interfacial contact; battery performance

Funding

  1. National Key Research and Development Program of China [2018YFE0124500, 2019YFA0705700]
  2. National Science Fund for Distinguished Young Scholars [51825102]
  3. National Natural Science Foundation of China [U1804255]

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Hybrid solid/gel electrolytes (SGEs) have attracted much attention for their ability to suppress Li dendrite growth and enhance battery safety, but the interfacial compatibility of electrode/electrolyte or polymer/inorganic ceramics within hybrid electrolytes remains a challenge. In this study, a hierarchical layered SGE was successfully fabricated by confining ceramic particles (LLZO) into G4-based gel electrolytes, demonstrating promising potential for high-performance Li-metal batteries.
Hybrid solid/gel electrolytes (SGEs) have generated much research attentions because of their capability to suppress Li dendrite growth and improve battery safety. However, the interfacial compatibility of the electrode/electrolyte or polymer/inorganic ceramics within hybrid electrolytes remains challenging for practical applications. Herein, an SGE is fabricated by confining ceramic particles (Li7La3Zr2O12; LLZO) into in situ formed tetraethylene glycol dimethyl ether (G4)-based gel electrolytes within assembled cells. A hierarchical layered structure is formed when LLZO settles near the Li anode within the liquid electrolyte during the gradual gelatinization process. Good interfacial compatibility is obtained from good contact with the liquid G4 component. The LLZO layer also serves as an ionic sieve to redistribute the Li deposition. This SGE endows stable Li stripping/plating cycling over 800 h at 0.5 mA/cm(2) (60 degrees C). Moreover, Li-metal batteries with an SGE coupled with LiFePO4 and an air cathode both exhibit superior cycling performance. This work presents a promising strategy for hierarchically layered SGEs for high-performance Li-metal batteries.

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