Heterocyclic Conjugated Polymer Nanoarchitectonics with Synergistic Redox-Active Sites for High-Performance Aluminium Organic Batteries

Xiyue Peng, Yuan Xie, Ardeshir Baktash, Jiayong Tang, Tongen Lin, Xia Huang, Yuxiang Hu, Zhongfan Jia, Debra J. Searles, Yusuke Yamauchi, Lianzhou Wang, Bin Luo

Research output: Contribution to journalArticlepeer-review

10 Citations (Scopus)
6 Downloads (Pure)

Abstract

The development of cost-effective and long-life rechargeable aluminium ion batteries (AIBs) shows promising prospects for sustainable energy storage applications. Here, we report a heteroatom π-conjugated polymer featuring synergistic C=O and C=N active centres as a new cathode material in AIBs using a low-cost AlCl3/urea electrolyte. Density functional theory (DFT) calculations reveal the fused C=N sites in the polymer not only benefit good π-conjugation but also enhance the redox reactivity of C=O sites, which enables the polymer to accommodate four AlCl2(urea)2+ per repeating unit. By integrating the polymer with carbon nanotubes, the hybrid cathode exhibits a high discharge capacity and a long cycle life (295 mAh g−1 at 0.1 A g−1 and 85 mAh g−1 at 1 A g−1 over 4000 cycles). The achieved specific energy density of 413 Wh kg−1 outperforms most Al–organic batteries reported to date. The synergistic redox-active sites strategy sheds light on the rational design of organic electrode materials.

Original languageEnglish
Article numbere202203646
Number of pages10
JournalAngewandte Chemie - International Edition
Volume61
Issue number25
Early online date24 Mar 2022
DOIs
Publication statusPublished - 20 Jun 2022

Keywords

  • AlCl/Urea Electrolyte
  • Aluminium Batteries
  • Heterocycles
  • Polymer Electrodes
  • Redox Chemistry

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