Donor‐Π‐Acceptor Self‐Adaptive Conjugated Perylene Derivative with Low Solubility, High Capacity, and Swift Ion Transport Kinetics for High Performance Organic Cathode

Organic perylene has been heralded as a promising candidate due to abundant structural diversity and tunability. However, its practical application is severely plagued by facile solubility, scarce redox-active sites, and andante kinetics behaviors. Herein, the perylene derivative (DPL), i.e., (1,6,7,12-tetrakis (4-tert-butylphenoxy) perylene-3,4,9,10-tetracarboxylic dianhydride) conjugates with polyoxime ester (PO) and is further nested with N, P grafted hollow matrix with anchored Cu single atoms (Cu-NPC). Such Cu-NPC@DPL@PO with helically twisted donor-π-acceptor (D-π-A) conjugate bridged by Cu atoms was evaluated for K⁺ storage. Based on extended π-π conjugated structure, intensified interactions between PO and DPL, the minimal solubility of DPL is approached. Together with the core-shell solvation structure and compact cathode electrolyte interface (CEI) synergistically improves its long lifespan. The abundant stabled radical nitroxides, isocyano groups, and sp-C sites contribute greatly to the capacity elevation. The twisted D-π-A self-adaptive coordination conjugate (TSCC) significantly elevates the distortion toward for the easier tendency to flipping and vibrating and thus expedited kinetics behaviors. Consequently, Cu-NPC@DPL@PO reconciles the trade-off between fast-charging and long cycle stability involved 8-electron participation. This work exemplifies the importance of advanced design of the molecular scale engineering, including modulated redox-active sites and high stability toward for fast-charging and long-lifespan cell devices.