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Diluent-Reorganized Solvation Structure for High-Voltage Lithium Metal Batteries
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张
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DOI：10.34133/energymatadv.0249.png)
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Abstract
En 中文
Localized high-concentration electrolytes (LHCEs) demonstrate promising performance in high-voltage lithium (Li) metal batteries. However, the understanding of Li+ migration kinetics and solvation configuration controlled by diluents is still lacking, limiting LHCEs’ rational design and optimization. In this study, we establish the structure–activity relationship between diluent-concentration-controlled Li+-solvated structures and kinetic signatures in LHCEs. Specifically, diluent concentration optimization reveals a volcano-type relationship in LHCE performance: Li+ transport kinetics and interfacial stability first improve (0 vol.% → 50 vol.%) due to enhanced dipole-mediated solvation reorganization and then degrade (50 vol.% → 75 vol.%) from excessive Li+ channel disruption. Consequently, an LHCE with 50 vol.% diluent achieves optimal kinetics and interfacial stability, enabling Li||Li cells to cycle stably over 4,500 h at 0.5 mA cm−2 with 25-mV voltage polarization. Furthermore, 4.6-V Li||LiCoO2 cells achieve 800 cycles at 2C (63% retention) while maintaining 129.7 mAh g−1 at 5C. These findings reveal the critical role of diluents in LHCE design, highlighting the promise of LHCEs for high-voltage lithium metal battery applications.
Keywords:
Lithium metal batteries
Localized high-concentration electrolytes
Solvation structure
Li+ migration kinetics
Diluent concentration
Journal
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15.9
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225
Citations:
1.6K
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