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Summary: The application of conducting polymers (CPs) in energy storage systems is greatly limited by insufficient reversibility and stability. Here, we successfully incorporated functionalized dopants (Fe(CN)63− [FCN] and PO43− ions) in CPs matrixes to achieve a preferable electrochemical performance. A stable cation inserting/expulsing behavior of surface-doped polycarbazole (PCz) is demonstrated in our work, where doping levels and semiconductor properties of PCz are effectively controlled to adjust their redox properties and stability. With carbon nanotube (CNT) films as the substrate, the CNT/PCz:FCN composite is initially adopted as a free-standing catalytic electrode in Li-O2 cells. The molecule-level dispersed FCN dopants on the surface can work as bifunctional redox mediators on the charge-discharge process. Thus, this composite can not only achieve a low charge plateau of 3.62 V and a regular growth of capacities from 1,800 to 4,800 mAh/gCNT, but also maintain the most of charge voltages under 4.0 V for 150 cycles. : Catalysis; Energy Storage; Polymers Subject Areas: Catalysis, Energy Storage, Polymers

Summary The application of conducting polymers (CPs) in energy storage systems is greatly limited by insufficient reversibility and stability. Here, we successfully incorporated functionalized dopants (Fe(CN)63− [FCN] and PO43− ions) in CPs matrixes to achieve a preferable electrochemical performance. A stable cation inserting/expulsing behavior of surface-doped polycarbazole (PCz) is demonstrated in our work, where doping levels and semiconductor properties of PCz are effectively controlled to adjust their redox properties and stability. With carbon nanotube (CNT) films as the substrate, the CNT/PCz:FCN composite is initially adopted as a free-standing catalytic electrode in Li-O2 cells. The molecule-level dispersed FCN dopants on the surface can work as bifunctional redox mediators on the charge-discharge process. Thus, this composite can not only achieve a low charge plateau of 3.62 V and a regular growth of capacities from 1,800 to 4,800 mAh/gCNT, but also maintain the most of charge voltages under 4.0 V for 150 cycles., Graphical Abstract, Highlights • A controllable electrochemical method to introduce redox-active anions in CP matrixes • Doping levels and semiconductor properties of CPs can be effectively controlled • Surface-doped CPs have better redox properties and electrochemical stability • The PCz doped by functionalized dopants shows a good catalytic effect, Catalysis; Energy Storage; Polymers