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Grain Boundary Engineering in Ta-Doped Garnet-Type Electrolyte for Lithium Dendrite Suppression
Zhiwei Qin1, Yuming Xie1, Xiangchen Meng1
1State Key Laboratory of Advanced Welding and Joining, Harbin Institute of Technology, Harbin 150001, China.
ACS Applied Materials & Interfaces
|September 1, 2022
Summary
Solid-state lithium batteries with Ta-doped LLZTO electrolytes face dendrite issues. Grain boundary engineering using La2O3 additive successfully suppressed dendrites and improved battery performance.
Area of Science:
- Materials Science
- Electrochemistry
- Solid-state Chemistry
Background:
- Solid-state lithium batteries (SSLBs) are promising for safer energy storage.
- Ta-doped Li6.5La3Zr1.5Ta0.5O12 (LLZTO) electrolytes are susceptible to lithium dendrite growth, limiting their practical use.
- Lithium dendrites compromise battery safety and performance.
Purpose of the Study:
- To investigate the mechanism of Ta segregation in LLZTO.
- To enhance the density and stability of LLZTO electrolytes through grain boundary engineering.
- To suppress lithium dendrite growth in SSLBs.
Main Methods:
- First principles simulations to analyze Ta doping effects.
- Introduction of La2O3 as an additive for grain boundary engineering.
- Fabrication and electrochemical testing of LLZTO-based solid-state electrolytes and batteries.
Main Results:
- First principles simulations revealed Ta segregation as Ta2O5 precipitates at grain boundaries.
- LLZTO + 5 wt% La2O3 achieved ~98% relative density with homogeneous Ta distribution.
- Critical current density increased by 41% to 2.12 mA·cm-2.
- SSLBs demonstrated stable cycling with 138.6 mA·h·g-1 discharge capacity after 400 cycles.
Conclusions:
- Grain boundary engineering with La2O3 effectively mitigates Ta segregation and enhances LLZTO density.
- The modified LLZTO electrolyte significantly improves critical current density and suppresses lithium dendrites.
- This approach offers a viable strategy for developing high-performance and safe solid-state lithium batteries.
