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

doi:10.1002/anie.202203646

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

Angew Chem Int Ed Engl. 2022 Jun 20;61(25):e202203646. doi: 10.1002/anie.202203646. Epub 2022 Apr 13.

Authors

Xiyue Peng¹, Yuan Xie¹, Ardeshir Baktash^{1

2}, Jiayong Tang^{1

2}, Tongen Lin^{1

2}, Xia Huang^{1

2}, Yuxiang Hu³, Zhongfan Jia⁴, Debra J Searles^{1

5}, Yusuke Yamauchi^{1

2}, Lianzhou Wang^{1

2}, Bin Luo¹

Affiliations

¹ Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, St. Lucia, QLD, 4072, Australia.
² School of Chemical Engineering, The University of Queensland, St. Lucia, QLD, 4072, Australia.
³ Key Laboratory of Advanced Functional Materials of Education Ministry of China, Faculty of Engineering and Manufacturing, Beijing University of Technology, Beijing, 100124, China.
⁴ Institute for Nanoscale Science and Technology, College of Science and Engineering, Flinders University, Bedford Park, South Australia, 5042, Australia.
⁵ School of Chemistry and Molecular Biosciences, The University of Queensland, St, Lucia, QLD, 4072, Australia.

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.

Keywords: AlCl3/Urea Electrolyte; Aluminium Batteries; Heterocycles; Polymer Electrodes; Redox Chemistry.

Abstract

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