High‐Cycling Performance of Viologen‐Based Conjugated Ionic Porous Organic Polymer Anode for Li‐Ion Batteries

ABSTRACT Compounds based on viologen are of great interest as anodes in lithium‐ion batteries (LIBs) due to their π‐conjugated aromatic structures, abundant active sites that promote stronger redox activity, and excellent structural tunability. In this study, two novel conjugated porous organic polymers, BIP‐TAA and DPT‐TAA, are synthesized via the Zincke reaction using different viologen structures as monomers. The electrochemical performance of BIP‐TAA and DPT‐TAA as anodes in lithium‐ion batteries is then investigated. Compared to BIP‐TAA, DPT‐TAA demonstrates superior electrochemical performance, including higher electrical conductivity and enhanced redox activity, owing to the introduction of the bithiazole ring that extends the π‐conjugated structure. Specifically, at a high current density of 2000 mA g −1 , DPT‐TAA delivers a capacity of 113.67 mAh g −1 , immediately highlighting its advantages. More importantly, prolonged cycling at an identical rate increases the specific capacity of DPT‐TAA from 124.26 to 321.1 mAh g −1 , significantly outperforming BIP‐TAA (104.25 to 186.5 mAh g −1 ). This performance unequivocally validates that the rigid, conjugated structure of DPT‐TAA is pivotal for achieving outstanding cycling stability and capacity retention. Overall, DPT‐TAA outperforms the basic viologen polymer in terms of cycling stability and multiplicity performance, providing a promising direction for the development of high‐performance organic anode materials.