<p>While p-type intrinsically stretchable conjugated polymers have seen substantial progress, their n-type counterparts still exhibit substantially inferior performances. This work demonstrates the enhancement of the mechanical performances of high-mobility n-type conjugated polymers by tailoring side chain order, inspired by the molecular characteristics of oleic acid and stearic acid. With additional increasing side chain disorders resulting from the <i>cis</i>-configuration of the olefin structure, the tensile modulus of polymer films is reduced, and the crack-onset strain limits are increased. Accordingly, we successfully developed an intrinsically stretchable n-type polymer that retains high electron mobilities of ~0.4 cm<sup>2 </sup>V<sup>−1</sup> s<sup>−1</sup> under 50% strain or after 2000 stretching-releasing cycles at 25% strain. Furthermore, we investigate how polymer chain rearrangement influences the dynamic behavior of these polymers. Their stretchability is attributed to multiscale chain alignment during deformation, revealing a clear structure–performance relationship at the molecular level. In summary, our side-chain engineering approach provides a valuable design strategy for developing high-performance stretchable n-type conjugated polymers.</p>

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Achieving intrinsically stretchable high-performance n-type semiconducting polymers by tuning side chain ordering inspired by oleic acid

  • Xiao-Yan Zhang,
  • Zi-Di Yu,
  • Nai-Fu Liu,
  • Wenxi Sun,
  • Xin-Yi Wang,
  • Junjiang Wu,
  • Jintao Feng,
  • Yang-Kun Qu,
  • Si-Lu Li,
  • Zhi-Hao Xie,
  • Yu-Ze Sun,
  • Wan-Yun Hsieh,
  • Chen-Kai Pan,
  • Long Ye,
  • Ze-Fan Yao,
  • Jie-Yu Wang,
  • Jian Pei

摘要

While p-type intrinsically stretchable conjugated polymers have seen substantial progress, their n-type counterparts still exhibit substantially inferior performances. This work demonstrates the enhancement of the mechanical performances of high-mobility n-type conjugated polymers by tailoring side chain order, inspired by the molecular characteristics of oleic acid and stearic acid. With additional increasing side chain disorders resulting from the cis-configuration of the olefin structure, the tensile modulus of polymer films is reduced, and the crack-onset strain limits are increased. Accordingly, we successfully developed an intrinsically stretchable n-type polymer that retains high electron mobilities of ~0.4 cm2 V−1 s−1 under 50% strain or after 2000 stretching-releasing cycles at 25% strain. Furthermore, we investigate how polymer chain rearrangement influences the dynamic behavior of these polymers. Their stretchability is attributed to multiscale chain alignment during deformation, revealing a clear structure–performance relationship at the molecular level. In summary, our side-chain engineering approach provides a valuable design strategy for developing high-performance stretchable n-type conjugated polymers.