Hypercrosslinked Porous Organic Polymers from Tetraaniline and Anthraquinone for High-capacitance, Long-life Supercapacitors
摘要
Hypercrosslinked polymers (HCPs) are promising electrode materials for supercapacitors owing to their rigid three-dimensional networks and excellent structural stability; however, their electrochemical performance is often limited by an over-reliance on electric double-layer capacitance or insufficient redox-active sites. Herein, we report a series of hypercrosslinked polymers (HCPs) constructed from tetraaniline (TANI) and 2,6-diaminoanthraquinone (DAQ) to integrate abundant redox-active sites with robust three-dimensional porous networks for high-capacitance and long-life supercapacitor electrodes. By tuning the TANI-to-DAQ molar ratio, the optimized TADA11-HCP exhibits a hierarchical micro-/mesoporous architecture for exposed active sites and facilitated mass diffusion, along with the lowest optical bandgap (acid-treated) among the series for fast electron transport. Benefiting from the combined advantages of structural strength, hierarchical porosity, and an optimized electronic structure, TADA11-HCP achieves 700 F·g−1 at 1 A·g−1 and retains 92% capacitance after 10000 cycles, demonstrating excellent cycling stability. A flexible quasi-solid-state symmetric supercapacitor further demonstrates 278.4 F·g−1 and an energy density of 38.7 Wh·kg−1, highlighting the practical potential of TADA-HCPs for advanced supercapacitor applications. This work demonstrates an effective molecular-level strategy to enhance the capacitance of HCP-based electrodes while maintaining long-term stability, providing insights into the rational design of high-performance HCPs for supercapacitor applications.