High-Voltage Recyclable Organic Cathode Enabled by Heteroatomic Substitution for Aqueous Zinc-Ion Batteries

Dawei Du, Jiyao Zhou, Zilong Yin, Guanzheng Feng, Weixiao Ji*, He Huang*, Siping Pang*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

4 Citations (Scopus)

Abstract

N-type organic compounds present themselves as promising high-capacity cathodes for aqueous Zn-ion batteries. However, a common challenge is their working voltages often falling below 1 V versus Zn2+/Zn. To bridge this gap, a high-voltage organic material is first developed, 5,6,11,12-tetraazanaphthacene (TANC), using a heteroatomic substitution strategy. TANC feature a large π-conjugated plane enriched with π−π interactions, which not only enhancing structural stability but also boosting charge transfer kinetics. The TANC cathode is achieved from its dihydro precursor, denoted as 2H-TANC, via a facile in situ activation process within the battery itself. This electrochemical synthesis method is cost-effective and environmentally friendly compared to traditional chemical method. The cathode shows a record-high discharge voltage of 1.15 V (vs Zn2+/Zn) among n-type organic materials and maintains cycling stability over 47,500 cycles. Furthermore, spent TANC electrodes can be efficiently recycled via a simple extraction process. The work marks a significant step toward the development of high-voltage, affordable, and recyclable organic electrode materials, steering them to the forefront of future sustainable battery technologies.

Original languageEnglish
Article number2400580
JournalAdvanced Energy Materials
Volume14
Issue number21
DOIs
Publication statusPublished - 5 Jun 2024

Keywords

  • aqueous Zn-ion batteries
  • heteroatomic substitution
  • high voltage
  • organic electrode materials
  • recyclability

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