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Garnet-Based Solid Li-Metal Batteries Operable under High External Pressure with HCOOH-Induced Electron-Blocking and
Haoyu Zhao1, Mingjie Du1, Haoran Mo1
1State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
ACS Applied Materials & Interfaces
|August 15, 2024
Summary
Formic acid treatment creates an electron-blocking layer on garnet solid electrolytes, improving lithium metal battery performance. This eco-friendly method enhances stability and reduces interfacial resistance for safer, long-lasting batteries.
Area of Science:
- Materials Science
- Electrochemistry
- Solid-State Chemistry
Background:
- Garnet solid electrolytes offer good compatibility with lithium metal.
- Challenges include electron-attack-induced lithium penetration and high interfacial resistance.
Purpose of the Study:
- To develop an eco-friendly method for enhancing garnet solid electrolytes.
- To improve the interfacial properties of lithium metal batteries.
Main Methods:
- Created an electron-blocking and lithiophilic interlayer using formic acid (HCOOH).
- Utilized a spontaneous reaction with surface Li2CO3 contamination on LLZTO.
- Employed a volatile, recyclable small-molecule organic acid.
Main Results:
- Achieved low interfacial impedance (3 Ω cm²) and high critical current density (1.7 mA cm⁻²).
- Demonstrated stable cycling for over 1000 hours at 0.2 mA cm⁻².
- Enabled stable lithium plating/stripping under pressure (2 MPa) at 0.3 mA cm⁻².
- LiFePO4//LLZTO cells maintained 88.5% capacity after 500 cycles.
Conclusions:
- Formic acid treatment is an effective, environmentally friendly strategy for interfacial engineering in garnet solid electrolytes.
- This method significantly enhances the performance and stability of solid lithium-metal batteries.
