期刊
ADVANCED MATERIALS INTERFACES
卷 7, 期 19, 页码 -出版社
WILEY
DOI: 10.1002/admi.202000751
关键词
Li10GeP2S12(LGPS); mechanical failure; solid electrolytes; solvates; X-ray tomography
资金
- Center for Electrochemical Energy Science, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Science
- DOE Office of Science [DE-AC02-06CH11357]
- National Science Foundation Graduate Research Fellowship Program [DGE-1144245]
Herein, the mechanical behaviors of Li10GeP2S12(LGPS) solid electrolytes during electrochemical cycling using operando X-ray tomography are investigated. It is demonstrated that the bulk mechanical decomposition of LGPS when cycled against lithium is a direct result of electrochemical reduction of the solid electrolyte at the LGPS/Li(0)interface. The reductive decomposition of LGPS during lithium plating results in the formation of low-density domains at the electrode/electrolyte interface, which impose sufficient mechanical stress on the underlying LGPS to crack the SE pellet. The critical stress developed prior to pellet fracture is significantly lower than the bulk shear modulus of LGPS, suggesting that the electrochemical instability of LGPS dramatically worsens the mechanical stability of the material near the LGPS/Li(0)interface. It is also shown that the application of a highly concentrated liquid electrolyte to the LGPS surface suppresses the reductive decomposition of LGPS, improving both the electrochemical performance and mechanical stability of the bulk LGPS solid electrolyte.
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