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Abstract Matching the capacity of the anode and cathode is essential for maximizing electrochemical cell performance. This study presents two strategies to balance the electrode utilization in zinc ion supercapacitors, by decreasing dendritic loss in the zinc anode while increasing the capacity of the activated carbon cathode. The anode current collector was modified with copper nanoparticles to direct zinc plating orientation and minimize dendrite formation, improving the Coulombic efficiency and cycle life. The cathode was activated by an electrolyte reaction to increase its porosity and gravimetric capacity. The full cell delivered a specific energy of 192 ± 0.56 Wh kg⁻¹at a specific power of 1.4 kW kg⁻¹, maintaining 84% capacity after 50,000 full charge-discharge cycles up to 2 V. With a cumulative capacity of 19.8 Ah cm⁻²surpassing zinc ion batteries, this device design is particularly promising for high-endurance applications, including un-interruptible power supplies and energy-harvesting systems that demand frequent cycling. 

Structural supercapacitors reach high performance with a gradient electrolyte and redox polymer electrodes. 

Ladder-type structures can impart exceptional stability to polymeric electronic materials. This article introduces a new class of conductive polymers featuring a fully ladder-type backbone. A judicious molecular design strategy enables the synthesis of a low-defect ladder polymer, which can be efficiently oxidized and acid-doped to achieve its conductive state. The structural elucidation of this polymer and the characterization of its open-shell nature are facilitated with the assistance of studies on small molecular models. An autonomous robotic system is used to optimize the conductivity of the polymer thin film, achieving over 7 mS cm^−1. Impressively, this polymer demonstrates unparalleled stability in strong acid and under harsh UV-irradiation, significantly surpassing commercial benchmarks like PEDOT:PSS and polyaniline. Moreover, it displays superior durability across numerous redox cycles as the active material in an electrochromic device and as the pseudocapacitive material in a supercapacitor device. This work provides structural design guidance for durable conductive polymers for long-term device operation.