Conducting polymers (CPs) constitute a promising building block to establish next‐generation stretchable electronics. However, achieving CPs with both high electrical conductivity and outstanding mechanical stretchability beyond flexibility is still a major challenge. Therefore, understanding the key factors controlling such characteristics of CPs is required. Herein, a method to simultaneously manipulate the mechanical and electrical properties of a representative CP, PEDOT:PSS, by modifying ionic liquid (IL) additives is reported. The cation/anion modification of ILs distinctly improves the electrical conductivity of PEDOT:PSS up to ≈1075 S cm⁻¹, and the PEDOT:PSS/IL films showing higher conductivity also exhibit superior electromechanical stretchability, enabling them to maintain their initial conductivity under a tensile strain of 80%. Based on grazing incidence wide angle X‐ray scattering and Fourier transform infrared spectroscopy analyses, it is found that the cation/anion‐modified ILs control the crystallinity and π–π stacking density of conjugated PEDOT chains and the growth of amorphous PSS domains via IL‐induced phase separation between PEDOT and PSS, which can be the origin of the significant conductivity and stretchability improvements in PEDOT:PSS/IL composites. This study provides guidance to develop highly stretchable CP‐based conductors/electrodes.

中文翻译：

---

调整可拉伸PEDOT：PSS /离子液体导体的机械和电气性能

导电聚合物（CPs）是建立下一代可拉伸电子产品的有希望的基础。然而，要获得具有高电导率和出色的机械拉伸性（不仅限于柔韧性）的CP，仍然是一项重大挑战。因此，需要了解控制CP的此类特性的关键因素。本文中，报告了一种通过改性离子液体（IL）添加剂来同时控制代表性CP PEDOT：PSS的机械和电气性能的方法。IL的阳离子/阴离子修饰可明显提高PEDOT：PSS的电导率，最高可达≈1075S cm ^-1，并且显示出更高电导率的PEDOT：PSS / IL膜也显示出优异的机电拉伸性，从而使它们能够在80％的拉伸应变下保持其初始电导率。基于掠入射的广角X射线散射和傅立叶变换红外光谱分析，发现阳离子/阴离子修饰的离子液体控制共轭PEDOT链的结晶度和π–π堆积密度，以及通过离子液体生长无定形PSS结构域导致PEDOT和PSS之间发生相分离，这可能是PEDOT：PSS / IL复合材料电导率和可拉伸性显着提高的原因。这项研究为开发高度可拉伸的基于CP的导体/电极提供了指导。