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Solid-State Lithium Batteries with Ultrastable Cyclability: An Internal-External Modification Strategy
Linshan Luo1, Zhefei Sun2, Yiwei You1
1Key Laboratory of Low Dimensional Condensed Matter Physics (Department of Education of Fujian Province), College of Physical Science and Technology, Xiamen University, Xiamen 361005, China.
ACS Nano
|January 15, 2024
Summary
Introducing a dual modification strategy, this study stabilizes lithium-ion battery interfaces by addressing defects in lithium aluminum titanium phosphate (LATP) and protecting the lithium metal anode. This enhances battery longevity and performance under demanding conditions.
Area of Science:
- Materials Science
- Electrochemistry
- Solid-State Batteries
Background:
- The interface between lithium aluminum titanium phosphate (LATP) solid electrolytes and lithium metal anodes presents stability challenges, limiting battery performance.
- Existing interlayer strategies show limited effectiveness in long-term cycling and high current density due to unaddressed internal LATP defects like grain boundaries (GBs).
- Grain boundaries in LATP exhibit higher electronic conductivity, promoting detrimental side reactions with lithium.
Purpose of the Study:
- To investigate the role of LATP grain boundaries in interfacial instability with lithium metal.
- To develop a dual modification strategy for stabilizing the LATP/lithium interface.
- To enhance the cycling stability and safety of solid-state lithium metal batteries.
Main Methods:
- Control experiments and theoretical calculations to analyze LATP grain boundary properties.
- LiCl solution immersion method to modify grain boundary electronic states.
- Composite solid polymer electrolyte (CSPE) interlayering at the Li/LATP interface.
- Fabrication and electrochemical testing of modified lithium symmetrical cells.
Main Results:
- LiCl treatment effectively modifies LATP grain boundaries, reducing their electronic conductivity and side reactions with lithium.
- The combined LiCl treatment and CSPE interlayering provide internal and external protection to the LATP electrolyte.
- Modified cells demonstrate ultrastable cycling performance, exceeding 3500 hours at 0.4 mA cm⁻² and 1500 hours at 0.6 mA cm⁻².
- The dual modification strategy effectively inhibits electron leakage, prevents side reactions, and suppresses lithium dendrite penetration.
Conclusions:
- Addressing internal defects, specifically grain boundaries, is crucial for stabilizing LATP electrolytes.
- A dual modification approach combining LiCl treatment and CSPE interlayering offers a highly effective strategy for interfacial stabilization.
- This method significantly improves the long-term cycling performance and reliability of solid-state lithium metal batteries.

