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Electron Percolating Shielded Interlayer Enabling Ultrastable All-Solid-State Lithium Metal Batteries.

Yang Zhao1, Yuetao Ma1, Jun Yang1

  • 1Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center, Institute of Materials Research (IMR), Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, P. R. China.

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Summary
This summary is machine-generated.

A novel interface strategy using Poly[bis(4-phenyl)(2,4,6-triMethylphenyl)aMine] (PTAA)/SnO2 (PS) bilayer effectively suppresses lithium dendrite growth in Li6.4La3Zr1.4Ta0.6O12 (LLZTO) solid-state batteries. This enhances stability and cycling performance for practical applications.

Keywords:
LLZTOinterface optimizationinterfacial electric fieldsolid‐state lithium metal batteries

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Batteries

Background:

  • Electron percolation in Li6.4La3Zr1.4Ta0.6O12 (LLZTO) grain boundaries causes internal lithium deposition and short circuits.
  • This significantly hinders the practical application of LLZTO in all-solid-state batteries.

Purpose of the Study:

  • To propose an electron-percolating shielded interface construction strategy between LLZTO and lithium metal (Li).
  • To suppress Li dendrite growth at the interface and within the LLZTO electrolyte.
  • To enhance the performance and durability of garnet-based all-solid-state lithium-metal batteries.

Main Methods:

  • Designed a Poly[bis(4-phenyl)(2,4,6-triMethylphenyl)aMine] (PTAA)/SnO2 (PS) bilayer interface (LLZTO-PS|Li).
  • Utilized the reverse electric field generated by PTAA and SnO2 to block electron leakage and reduce LLZTO electronic conductivity.
  • Applied a smooth and compact PTAA/SnO2 coating to enhance interfacial contact and promote uniform Li plating.

Main Results:

  • The Li|LLZTO-PS|Li symmetric battery achieved stable cycling over 5000 hours at 0.1 mA cm⁻² and 2500 hours at 0.5 mA cm⁻².
  • The Li|LLZTO-PS|LiFePO4 full battery retained 86.2% capacity after 2000 cycles at 1 C.
  • Demonstrated effective suppression of internal dendrite formation and uniform Li plating.

Conclusions:

  • The PTAA/SnO2 bilayer interface strategy effectively mitigates electron percolation issues in LLZTO.
  • This approach significantly enhances the electrochemical performance and long-term stability of solid-state lithium metal batteries.
  • Presents a viable solution for advancing garnet-based solid-state battery technology.