Tailored Stereo‐Configuration of Crosslinkable Polyester‐Based Solid Polymer Electrolytes for All‐Solid‐State and Binder‐Free Li Metal Batteries
Abstract
By harnessing stereoisomerism in unsaturated polyesters, we elucidate how subtle structural variations impact Li + solvation structures by modulating free volume, Li + diffusivity, and lithium salt dissociation within solid polymer electrolytes (SPEs). The intrinsic reactivity of C═C bonds along the polymeric backbones is further exploited via a facile UV‐curing approach to construct robust three‐dimensional polymeric networks that impart mechanical robustness and preferential restriction of TFSI − mobility relative to Li + transport. The distorted conformation of poly( n ‐pentyl maleate) (PPM) leads to sparsely crosslinked structures, preserving efficient Li + transport pathways. Furthermore, end‐group fluorination enhances interfacial stability by facilitating the formation of a LiF‐rich solid electrolyte interphase. These synergistic design strategies culminate in a crosslinked PPM‐based SPE (XL‐PPM‐3F‐Li) featuring one CF 3 end‐capping group, which exhibits remarkable electrochemical durability in both Li||Li symmetric and LFP full‐cell configurations. Furthermore, this advantage is extended to the device level by integrating binder, electrolyte, and separator into a single ultrathin (∼“5 µm‐thick”) crosslinked SPE that conformally interfaces with the electrode microstructure. This integrated configuration markedly lowers interfacial and charge‐transfer resistance, enabling 65% of the initial reversible capacity at 2 C and 93.6% retention after 100 cycles at 0.5 C (60°C). Overall, this crosslinking‐enabled unified architecture establishes a robust strategy for ultra‐stable solid‐state lithium‐metal batteries.
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BibTeX
@article{song2026tailored,
title = {{Tailored Stereo‐Configuration of Crosslinkable Polyester‐Based Solid Polymer Electrolytes for All‐Solid‐State and Binder‐Free Li Metal Batteries}},
author = {Hyun Jun Song and Jeong Yoon Kim and Sungpyo Hong and Yong Hui Kim and Myeong Gyun Nam and Jeong‐won Ho and Min Gi Kang and Hye Seon Kim and Chaeyeon Ha and Sang Uck Lee and Pil J Yoo and Patrice Rannou},
journal = {Advanced Science},
year = {2026},
month = aug,
doi = {10.1002/advs.202600063},
url = {https://hal.science/hal-05735707v1},
note = {CC BY 4.0},
}
RIS
TY - JOUR
TI - Tailored Stereo‐Configuration of Crosslinkable Polyester‐Based Solid Polymer Electrolytes for All‐Solid‐State and Binder‐Free Li Metal Batteries
AU - Hyun Jun Song
AU - Jeong Yoon Kim
AU - Sungpyo Hong
AU - Yong Hui Kim
AU - Myeong Gyun Nam
AU - Jeong‐won Ho
AU - Min Gi Kang
AU - Hye Seon Kim
AU - Chaeyeon Ha
AU - Sang Uck Lee
AU - Pil J Yoo
AU - Patrice Rannou
PY - 2026
DA - 2026/08/24
JO - Advanced Science
DO - 10.1002/advs.202600063
UR - https://hal.science/hal-05735707v1
AB - By harnessing stereoisomerism in unsaturated polyesters, we elucidate how subtle structural variations impact Li + solvation structures by modulating free volume, Li + diffusivity, and lithium salt dissociation within solid polymer electrolytes (SPEs). The intrinsic reactivity of C═C bonds along the polymeric backbones is further exploited via a facile UV‐curing approach to construct robust three‐dimensional polymeric networks that impart mechanical robustness and preferential restriction of TFSI − mobility relative to Li + transport. The distorted conformation of poly( n ‐pentyl maleate) (PPM) leads to sparsely crosslinked structures, preserving efficient Li + transport pathways. Furthermore, end‐group fluorination enhances interfacial stability by facilitating the formation of a LiF‐rich solid electrolyte interphase. These synergistic design strategies culminate in a crosslinked PPM‐based SPE (XL‐PPM‐3F‐Li) featuring one CF 3 end‐capping group, which exhibits remarkable electrochemical durability in both Li||Li symmetric and LFP full‐cell configurations. Furthermore, this advantage is extended to the device level by integrating binder, electrolyte, and separator into a single ultrathin (∼“5 µm‐thick”) crosslinked SPE that conformally interfaces with the electrode microstructure. This integrated configuration markedly lowers interfacial and charge‐transfer resistance, enabling 65% of the initial reversible capacity at 2 C and 93.6% retention after 100 cycles at 0.5 C (60°C). Overall, this crosslinking‐enabled unified architecture establishes a robust strategy for ultra‐stable solid‐state lithium‐metal batteries.
SN - 2198-3844
ER -