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Nanoscale Thermomechanical Coupling Study on the Aging of NASICON-Type Solid Electrolytes
Xuyang Wang1,2, Fang Wang1,2,3, Qingfeng Zhu4
1Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, Guangdong, China.
Nano Letters
|May 17, 2025
Summary
New research reveals that thermal properties significantly impact solid electrolyte aging. A secondary phase in Li1.4Al0.4Ti1.6(PO4)3 (LATP) solid electrolytes shows reduced thermal conductivity and mechanical stability, leading to battery degradation.
Area of Science:
- Materials Science
- Electrochemistry
- Nanotechnology
Background:
- Aging mechanisms of solid electrolytes (SEs) are typically studied through electrochemical and mechanical properties.
- Thermal characteristics of SEs during aging have been largely overlooked in previous research.
- Understanding SE degradation is crucial for developing advanced solid-state batteries.
Purpose of the Study:
- To investigate the microscopic aging process of Li1.4Al0.4Ti1.6(PO4)3 (LATP) solid electrolytes using advanced thermal microscopy techniques.
- To elucidate the role of thermomechanical coupling at the nanoscale in SE degradation.
- To identify the formation and properties of secondary phases during LATP SE cycling.
Main Methods:
- Utilized scanning thermal microscopy (SThM) and scanning thermo-ionic microscopy (STIM) to probe nanoscale thermal and ionic properties.
- Analyzed the Li1.4Al0.4Ti1.6(PO4)3 (LATP) solid electrolyte assembled with lithium metal.
- Characterized the formation of a secondary phase and its thermomechanical properties during cycling.
Main Results:
- Identified the formation of a Li3Al0.4Ti1.6(PO4)3 secondary phase during cycling of LATP SEs.
- Observed a significant decrease in thermal conductivity (1.72 to 0.63 W m-1 K-1) and Young's modulus (117.4 to 31.3 GPa) in the secondary phase.
- Noted increased thermal expansion and reduced ionic activity in the secondary phase, leading to interfacial issues, cracks, and impedance rise.
Conclusions:
- The study demonstrates the critical impact of thermomechanical coupling on solid electrolyte degradation at the nanoscale.
- The formation of a secondary phase with altered thermal and mechanical properties is a key factor in LATP SE aging.
- These findings highlight the necessity of considering thermal properties in the design and development of stable solid electrolytes for batteries.
