A Heavily Surface-Doped Polymer with the Bifunctional Catalytic Mechanism in Li-O2 Batteries.

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.