A COF‐Like N‐Rich Conjugated Microporous Polytriphenylamine Cathode with Pseudocapacitive Anion Storage Behavior for High‐Energy Aqueous Zinc Dual‐Ion Batteries

Abstract Conducting polymers with good electron conductivity and rich redox functional groups are promising cathode candidates for constructing high‐energy aqueous zinc batteries. However, the glaring flaw of active‐site underutilization impairs their electrochemical performance. Herein, we report a poriferous polytriphenylamine conjugated microporous polymer (CMP) cathode capable of accommodating Cl − anions in a pseudocapative‐dominated manner for energy storage. Its specific 3D, covalent‐organic‐framework‐like conjugated network ensures high accessibility efficacy of N active sites (up to 83.2% at 0.5 A g −1 ) and distinct physicochemical stability (87.6% capacity retention after 1000 cycles) during repeated charging/discharging courses. Such a robust CMP electrode also leads to a zinc dual‐ion battery device with a high energy density of 236 W h kg −1 and a maximum power density of 6.8 kW kg −1 , substantially surpassing most recently reported organic‐based zinc batteries. This study paves the way for the rational design of advanced CMP‐based organic cathodes for high‐energy devices.