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Regulating Incompatible Interfaces and Electron/Ion Transport in Lithium Metal Solid State Batteries.

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A novel Li2O/LixIn interface on LATP solid-state electrolytes enhances lithium-ion transfer and suppresses dendrites. This breakthrough significantly improves battery stability and performance, paving the way for advanced solid-state batteries.

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Li/LATP interfaceLi2O/LixIn layerelectron‐blockingfast ion transportlithiophilic

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Batteries

Background:

  • Large interfacial impedance and poor ion transport hinder LATP-based solid-state battery development.
  • Spontaneous reactions at the LATP/Li metal interface impede battery performance and safety.

Purpose of the Study:

  • To construct a fast Li+ transfer and electron-blocking interface on LATP.
  • To enhance the interfacial contact between LATP and Li metal.
  • To improve the electrochemical performance and stability of LATP-based solid-state batteries.

Main Methods:

  • In situ electrochemical reaction of In2O3 with Li metal to form a Li2O/LixIn interface on LATP.
  • Fabrication of Li/In2O3@LATP/Li symmetric batteries.
  • Testing of Li/In2O3@LATP/LiFePO4 and Li/In2O3@LATP/Li1.2Mn0.6Ni0.2O2 full batteries.

Main Results:

  • Reduced initial resistance from 1211.4 to 106.5 Ω cm-2.
  • Increased critical current density to 1.9 mA cm-2.
  • Stable cycling over 3700 h without dendrites at 0.2 mA cm-2/0.2 mAh cm-2.
  • Full battery with LiFePO4 cathode showed a decay rate of ≈0.015% per cycle after 600 cycles.
  • High voltage compatibility (4.8 V) with a nickel-manganese-cobalt cathode.

Conclusions:

  • The Li2O/LixIn interface effectively addresses interfacial issues in LATP solid-state batteries.
  • This interface promotes fast Li+ transport and suppresses Li dendrite growth.
  • The developed solid-state batteries exhibit excellent stability, high performance, and potential for practical applications.