Cross-linking enhances the performance of four-electron carbonylpyridinium based polymers for lithium organic batteries

Abstract

Design and integration of multiple redox-active organic scaffolds into tailored polymer structures to enhance the specific capacity and cycling life is a long-term research goal. Inspired by nature, we designed and incorporated a 4-electron accepting dicarbonylpyridinium redox motif into linear (DBMP) and cross-linked polymer (TBMP) structures. Benefiting from the suppressed solubility and higher electronic conductivity, the cross-linked TBMP based electrode exhibits improved cycling stability and higher specific capacity than the linear counterpart. After 4000 cycles at 1 A g⁻¹, TBMP can maintain a high capacity of 252 mA h g⁻¹, surpassing the performance of many reported organic cathodes. The structural evolution and reaction kinetics during charge and discharge have been investigated in detail. This study demonstrates that cross-linking is an effective strategy to push the bio-derived carbonylpyridinium materials for high performance LOBs.