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Hierarchical Primary-Secondary Coordination Synchronizes Ion Flux and Sulfur Redox in Solid Polymer Electrolytes
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DOI：10.1002/adfm.77192.png)
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Abstract
En 中文
Lithium-sulfur (Li-S) batteries suffer from transport-conversion imbalance, leading to concentration polarization, incomplete sulfur reduction, and unstable Li metal interfaces. Here, a coordination-engineered polymer electrolyte with a hierarchical primary-secondary Li+ coordination architecture is developed to synchronize ion transport and sulfur redox kinetics. A CO2-derived poly(propylene carbonate)-based ionic framework integrates crown ether primary coordination sites with distributed carbonate secondary motifs, promoting Li salt dissociation while sustaining dynamic Li+ migration. Spectroscopic and electrochemical analyses reveal redistributed Li+ solvation, weakened Li+-TFSI− association, and enhanced ionic conductivity on the order of 10−4 S cm−1, and a Li+ transference number of 0.45 at 60°C. The synchronized Li+ flux suppresses concentration polarization and stabilizes sulfur conversion and Li deposition. Solid-state Li-S cells with a sulfur loading of ≈2.0 mg cm−2 deliver an initial discharge capacity of 766 mAh g−1 and maintain ≈60% capacity retention during cycling at 0.1 C under liquid-electrolyte-free conditions. This work establishes hierarchical coordination engineering as a molecular strategy for coupling ion transport with redox conversion in solid-state battery systems.
Keywords:
hierarchical coordination
ion transport regulation
lithium-sulfur batteries
polymer electrolytes
polysulfide conversion
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