Flexible electrochromic supercapacitors (ECSCs) consisting of conjugated polymer electrodes are promising for integrating optical modulation with sustainable energy storage. However, there remain formidable challenges to achieving long-term cycling stability while maximizing high device output voltage. Here, we design a new twisted conjugated polymer bearing dual-redox centers (thiophene and triphenylamine) and an electron-withdrawing cyano group. The as-prepared conjugated polymer showcases elevated discharge potential and highly efficient charge transport synchronously, attributed to the lowered energy of the lowest unoccupied molecular (LUMO) orbitals and twisted alignment of the polymer chain. Coupled with the transparent vanadium pentoxide (V₂O₅) nanowires ion-storage material, the flexible ECSC affords a high optical contrast of 67 %, wide voltage window of 2 V, large capacitance of 32.9 mF/cm², and outstanding cycling durability (86 % capacitance and 96 % optical modulation retention after 7000 cycles at 0.2 mA/cm²). This molecular engineering strategy and insight illustrated by density functional theory (DFT) calculation together with electrochemical kinetics analysis provide another way along the route toward the synergetic improvement of electrochromic and energy storage performance.

由共轭聚合物电极组成的柔性电致变色超级电容器（ECSC）有望将光调制与可持续能量存储相结合。然而，要实现长期循环稳定性，同时最大限度地提高器件的高输出电压，仍然存在巨大的挑战。在这里，我们设计了一种带有双氧化还原中心（噻吩和三苯胺）和吸电子氰基的新型扭曲共轭聚合物。所制备的共轭聚合物同时表现出更高的放电电位和高效的电荷传输，这归因于最低未占分子 (LUMO) 轨道的能量降低和聚合物链的扭曲排列。再加上透明的五氧化二钒（V ₂ O ₅) 纳米线离子存储材料，柔性 ECSC 提供 67% 的高光学对比度、2 V 的宽电压窗口、32.9 mF/cm ²的大电容和出色的循环耐久性（86% 的电容和 96% 的光调制保留后在 0.2 mA/cm ²下循环 7000 次）。这种通过密度泛函理论 (DFT) 计算以及电化学动力学分析说明的分子工程策略和洞察力为协同改进电致变色和储能性能提供了另一种途径。