Heterocyclic Conjugated Polymer Nanoarchitectonics with Synergistic Redox‐Active Sites for High‐Performance Aluminium Organic Batteries. (13th April 2022)

• Record Type: Journal Article
• Authors: Peng, Xiyue; Xie, Yuan; Baktash, Ardeshir; Tang, Jiayong; Lin, Tongen; Huang, Xia; Hu, Yuxiang; Jia, Zhongfan; Searles, Debra J.; Yamauchi, Yusuke; Wang, Lianzhou; Luo, Bin
• Is Part Of: Angewandte Chemie. Volume 134:Number 25(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-04-13
• Subjects: AlCl3/Urea Electrolyte -- Aluminium Batteries -- Heterocycles -- Polymer Electrodes -- Redox Chemistry; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.202203646
• Languages: English
• ISSNs: 0044-8249

Abstract

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. Abstract : A synergistic C=O/C=N redox centre strategy has been demonstrated to realise high‐performance Al–organic batteries using a heteroatom π‐conjugated polymer cathode in a low‐cost AlCl3 /urea electrolyte. The fused C=N sites in the polymer not only contribute good π‐conjugation but also assist neighbouring C=O to uptake four AlCl2 (urea)2 + per repeating unit, enabling batteries with high capacity, long cyclability, and high energy density.