Interfacial Modification of All-Solid-State Lithium Metal Battery with Mixed Conductive Materials AITranslate

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Basic Information:

DOI：10.13373/j.cnki.cjrm.XY25040016

Chinese Library Classification Number:TM911

Citation Information:

Lithium （Li） metal anodes possess significant advantages in enhancing battery energy density due to their high theoretical specific capacity （3860 mAh·g⁻¹） and low potential （–3.04 V （vs. SHE））, meeting the requirements for high-energy-density batteries in the field of energy storage materials. Meanwhile, solid-state electrolytes （SEs） have become a research hotspot in the field of high-energy-density storage due to their outstanding advantages, including high safety and high energy density. Among them, sulfide solid-state electrolytes （SSEs） perform particularly well. Their ionic conductivity can approach that of liquid electrolytes （>1×10⁻³ S·cm⁻¹）, and they exhibit excellent mechanical properties. When matched with Li metal, they demonstrate good chemical stability. However, the growth problem of Li dendrite seriously restricts the further development of Li metal batteries. On one hand, Li dendrite triggers the decomposition reaction of electrolytes, generating a series of by-products. This not only reduces the stability of the electrolytes but also severely damages their chemical properties. On the other hand, Li dendrite has extremely strong penetrating power, which can cause cracks in the electrolytes and eventually penetrate them, leading to battery short circuits and posing significant safety hazards. Therefore, how to effectively inhibit the growth of Li dendrites remains one of the important challenges in the field of Li metal batteries. To address this issue, this study innovatively proposed to construct a mixed ion-electron conductive （MIEC） interfacial layer between SSEs and Li metal and systematically explored the mechanism by which this interfacial layer inhibited the growth of Li dendrites. Through precise regulation of the ionic and electronic conductivity properties of MIEC, it revealed that when the content of Super P （SP） was 1%, the electronic conductivity could be successfully optimized to 1.8×10⁻⁸ S·cm⁻¹ while maintaining high ionic conductivity. The performance of the symmetric cell prepared based on this had been significantly improved. The critical current density had been greatly increased to 1.6 mA·cm⁻², and it could stably cycle for up to 2800 h at a current density of 0.5 mA·cm⁻². In-depth analysis of the mechanism showed that 1%SP composite material constructed a three-dimensional ion-electron migration network in the interfacial layer, precisely optimizing the concentration distribution of Li ion migration and effectively inducing uniform deposition of Li ions. Analyses of the interfacial layer using X-ray diffraction （XRD） and scanning electron microscopy （SEM） confirmed that MIEC not only exhibited good contact performance but also showed a state of uniform Li metal deposition. In addition, the results of in-situ electrochemical impedance spectroscopy tests indicated that it could significantly reduce grain boundary impedance and effectively improved the charge transfer kinetics, making the electrochemical reactions inside the battery more efficient and stable. X-ray photoelectron spectroscopy （XPS） analysis further confirmed that MIEC still maintained high chemical stability after cycling, fully demonstrating the reliability of this interfacial layer. In the full-cell performance tests, the cell assembled with 1%SP interfacial layer exhibited excellent performance. Under the same rate test conditions, it showed higher discharge specific capacity, reaching 203 mAh·g⁻¹ at a rate of 0.1C. More importantly, at a rate of 1C, the full cell could stably cycle 1000 times with a capacity retention rate as high as 79.7%, fully demonstrating its excellent interfacial stability. In conclusion, this study successfully achieved a uniform distribution of the electric field by balancing the ionic/electronic conduction characteristics at MIEC between the electrolyte and Li metal, effectively inhibiting the nucleation and growth of Li dendrites. The research results provided new technical approaches and theoretical bases for the development of Li metal batteries and were expected to promote the widespread application of Li metal batteries in the field of energy storage.