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Direct Modeling of the Interfacial Resistance in All-Solid-State Battery
Da Wang1, Yaqiao Luo1, Jia Yu1
1State Key Laboratory of Materials for Advanced Nuclear Energy, School of Materials Science and Engineering, and Materials Genome Institute, Shanghai University, Shanghai, China.
Researchers developed a new method to accurately predict interfacial resistance in all-solid-state batteries (ASSBs) by directly mapping ion redistribution. This breakthrough reduces prediction errors and guides the selection of optimal materials for high-performance ASSBs.
Area of Science:
- Materials Science
- Electrochemistry
- Computational Modeling
Background:
- Interfacial resistance significantly impacts all-solid-state battery (ASSB) performance.
- Current methods for predicting interfacial resistance indirectly infer potentials, leading to large discrepancies with experimental data.
Purpose of the Study:
- To develop a non-empirical numerical procedure for directly mapping lithium-ion redistribution to interfacial resistance in ASSBs.
- To bridge the gap between theoretical modeling and experimental measurements of interfacial properties.
Main Methods:
- Integrated ligand-field theory with the space-charge layer (SCL) model.
- Developed a modified ligand-field splitting strength (MLFSS) descriptor to account for electric potential differences and carrier properties.
- Analyzed 310 distinct interfaces from extensive literature.
Main Results:
- Reduced predicted interfacial resistance discrepancies from over ten orders of magnitude to within two.
- Identified extreme MLFSS disparities (>3.5 eV) as the cause of high oxide interfacial resistance.
- Highlighted ion-intercalation sulfides (<0.2 eV) as promising cathodes due to intrinsic SCL suppression.
Conclusions:
- The developed MLFSS descriptor provides a tunable criterion for predicting and optimizing ASSB interfacial performance.
- Demonstrated the criterion's validity in an all-sulfide ASSB prototype with ultralow interfacial resistance (8.8 Ω cm²).
- Established a practical approach to overcome the energy-density and kinetics trade-off in ASSBs.
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