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<p>Helical-helical polypeptide polymerized ionic liquid block copolymers (PPIL BCPs) are synthesized to investigate the role of helical structure on self-assembly and ionic conductivity. PPIL BCPs, consisting of a cationic polypeptide (PTPLG) with bis(trifluoromethane sulfonimide) (TFSI) counterion and varying lengths connected to a length-fixed neutral poly-(γ-benzyl-<sub>L</sub>-glutamate) (PBLG) block, exhibit stable helical conformations with minimal glass transition (<i>T</i><sub>g</sub>) variation. Here, we show that increasing PIL composition leads to a transition from poorly ordered to highly ordered lamellar (LAM) structures with the highest PIL content BCP forming a bilayer LAM structure with close-packed helices. This morphology yields a 1.5 order of magnitude higher <i>T</i><sub>g</sub>- and volume fraction-normalized ionic conductivity and a morphology factor f &gt; 0.8 compared to less ordered BCPs with f &lt; 0.05 and f = 2/3 for ideal lamellae. These results highlight the critical role of helical structure in optimizing ion transport, offering a design strategy for high-performance solid electrolytes.</p>

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Ion transport in helical-helical polypeptide polymerized ionic liquid block copolymers

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年3月12日

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  • Yingying Chen,
  • Tianjian Yang,
  • Yao Lin,
  • Christopher M. Evans

摘要

Helical-helical polypeptide polymerized ionic liquid block copolymers (PPIL BCPs) are synthesized to investigate the role of helical structure on self-assembly and ionic conductivity. PPIL BCPs, consisting of a cationic polypeptide (PTPLG) with bis(trifluoromethane sulfonimide) (TFSI) counterion and varying lengths connected to a length-fixed neutral poly-(γ-benzyl-L-glutamate) (PBLG) block, exhibit stable helical conformations with minimal glass transition (Tg) variation. Here, we show that increasing PIL composition leads to a transition from poorly ordered to highly ordered lamellar (LAM) structures with the highest PIL content BCP forming a bilayer LAM structure with close-packed helices. This morphology yields a 1.5 order of magnitude higher Tg- and volume fraction-normalized ionic conductivity and a morphology factor f > 0.8 compared to less ordered BCPs with f < 0.05 and f = 2/3 for ideal lamellae. These results highlight the critical role of helical structure in optimizing ion transport, offering a design strategy for high-performance solid electrolytes.