Redox-Active High-Performance Polyimides as Versatile Electrode Materials for Organic Lithium- and Sodium-Ion Batteries

Organic electrode materials for rechargeable batteries show great promise for improving the storage capacity, reducing production costs, and minimizing environmental impact toward sustainability. In this study, we report a series of newly synthesized arylamine-based polyimides, TPPA-PIs, with three different bridge functionalizations on the imide rings and isomeric constituents that can work as versatile battery electrodes. As a lithium-ion battery cathode, a maximum energy density of 248 Wh kg-1 with high voltage operation up to 4.0 V can be achieved. As a lithium-ion battery anode, the TPPA-PIs showed a reversible storage capacity of 806 mA h g-1 at 100 mA g-1 current density with good rate capability up to a current density of 2000 mA g-1. Moreover, when applied as sodium-ion battery anodes, TPPA-PIs delivered an optimum specific capacity of up to 218 mA h g-1 after 50 cycles at a 50 mA g-1 current density and revealed a long cycling stability up to 1000 cycles under a high current density of 1000 mA g-1. More importantly, these electrochemical performances of TPPA-PIs are among the best compared with other reported polymer-based electrodes. The mechanistic studies show that both bridge functionalization on the imide units and isomerism impact the electrochemical performance by regulating their intrinsic properties such as charge storage behavior, ion diffusivity, and activation energy. We believe that such a detailed study of the structural design to electrochemical performance of these polymeric electrodes will offer insights into materials development and optimization for next-generation multifunctional energy storage devices in a wide range of applications.