ArticleJACS Au2026
From Brittle to Ultraductile: Precise Ionic PEG with Dynamic Networks and Reconfigurable Crystallites.
Article in JACS Au, 2026. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.
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Abstract
Achieving high ductility and toughness in semicrystalline polymers without sacrificing stiffness remains a longstanding challenge. Here we show that sparse precise ionic functionalization can fundamentally alter the mechanical behavior of a semicrystalline polymer. Ionic poly-(ethylene glycol) (iPEGs) containing precisely spaced imidazolium groups (∼1.5 mol %, every 62 repeat units) undergo a striking transition from brittle to ultraductile behavior, which exhibits stable neck propagation and apparent strain hardening at moderate molecular weight of 41 kDa. Tensile behavior, melt rheology, and X-ray scattering spectra reveal that this highly ductile behavior arises from a coupled ionic-semicrystalline architecture. Dynamic ionic associations introduce long-lived transient constraints that enhance the amorphous phase resistance to deformation and sustain load-bearing connectivity between crystallites, while ionic incorporation suppresses lamellar thickening and produces thin PEG crystallites capable of deformation-induced reorganization. The resulting interplay between crystallite connectivity, tie-chain load transfer, and reconfigurable crystallites enable stable neck propagation rather than brittle fracture. These results establish sparse ionic "stickers" as a molecular design principle for strengthening crystal-mobile semicrystalline polymers without introducing additional phases or permanent covalent cross-links.
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