TY  - JOUR
AU  - Wang, Tingting
AU  - Wang, Hao
AU  - Jia, Weishang
AU  - Zhang, Liwen
AU  - Jiao, Shuhong
AU  - Li, Hong
AU  - Wang, Liping
PY  - 2026
TI  - Diluent-Reorganized Solvation Structure for High-Voltage Lithium Metal Batteries
JO  - Energy Material Advances
SN  - 2097-1133
SP  - 0249
VL  - 7
AB  - 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.
UR  - https://doi.org/10.34133/energymatadv.0249
DO  - 10.34133/energymatadv.0249