Tunable Redox-Active Anhydride-Based Linear Polymer as Organic Cathodes for Chemically Self-Charging Aqueous Zinc–Ion Batteries AITranslate

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Chemically self-charging aqueous zinc-ion batteries (AZIBs) have emerged as promising candidates for energy storage technologies owing to their environmental autonomy and structural simplicity. Nonetheless, the self-charging performance is significantly compromised by the limited potential difference between cathodes and oxygen, as well as the unsatisfactory cycling stability. Herein, we synthesized three novel polymeric cathodes (PM-E, NT-E, and PT-E) derived from distinct anhydride precursors for application in both AZIBs and chemical self-charging AZIBs. Combined experimental and density functional theory (DFT) analyses indicate that the π-conjugated aromatic ring structures in various anhydride derivatives modulate the zinc storage activity of the carbonyl group (C=O). PT-E demonstrates superior electrochemical performance due to its optimal combination of band structure and molecular planarity, maintaining a specific capacity of 97.1 mAh g−1 at 1 A g−1 after 300 cycles for AZIBs. Particularly, the PT-E cathode exhibits rechargeability through direct air oxidation without the external power supply; the discharged chemical self-charging AZIBs can be recharged to 1.28 V after exposure to air for 12 h. Meanwhile, it demonstrates excellent compatibility with combined chemical/galvanostatic charging environments, exhibiting exceptional electrochemical reversibility. This study advances chemical self-charging AZIBs technology while expanding the utilization scope of organic materials in autonomous energy storage systems.