Self-Healing UPy-Functionalized Polyethylene Networks: A Robust Platform for Resilient and High-Performance Lithium Battery Separators.

Authors

Daniele Callegari, Arkadiusz Zych, Roberta Pinalli, Enrico Dalcanale, Eliana Quartarone

Published in

Advanced science (Weinheim, Baden-Wurttemberg, Germany). Pages e77850. Sep 27, 2026. Epub Sep 27, 2026.

Abstract

Conventional polyolefin separators exhibit limited mechanical resilience and poor damage tolerance, leading to performance degradation and critical safety concerns. To overcome these limitations, we developed supramolecular self-healing separators based on polyethylene-hydroxyethyl methacrylate (PE-HEMA) copolymers functionalized with ureidopyrimidinone (UPy) units. The UPy motifs undergo reversible dimerization through quadruple hydrogen bonding within the polymer matrix, forming a dynamic supramolecular network capable of autonomously repairing mechanical defects. Three copolymers with varying UPy grafting densities were synthesized and blended with high-molecular-weight polyethylene oxide (PEO) to significantly enhance electrolyte affinity and ionic transport. Composite membranes (35-40 µm) were subsequently produced via a rapid, solvent-free hot-pressing process. Due to increased amorphous character and enhanced polymer chain mobility, the resulting materials exhibit efficient self-healing at mild temperatures (40°C), improved electrolyte wettability, and high ionic conductivity. Electrochemical testing in Li|Li symmetric cells demonstrate that the separators successfully recover functionality after dendrite-induced short circuits through network reorganization. When implemented in LiFePO₄-based full cells, the optimized separator enables stable cycling, delivering a discharge capacity of ≈130 mAh g^{- 1} after 1000 cycles with up to 81.5% capacity retention, alongside improved thermal safety. These results highlight the promise of UPy-based supramolecular separators for next-generation lithium-based batteries.

PMID:
42801619
Bibliographic data and abstract were imported from PubMed on 28 Sep 2026.

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