Chinese Journal of Applied Chemistry ›› 2024, Vol. 41 ›› Issue (7): 998-1009.DOI: 10.19894/j.issn.1000-0518.240029

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Long-Term Aqueous Zinc-Ion Batteries without Dendrites Protected by Nitrogen Heterocyclic Imidazole Ionic Liquid

Lei XU1,2, Long-Yang WANG1,2, Li TAO1,2(), Hao-Nan ZHANG1,2, Xin-Wang JIA1,2, Hou-Zhao WAN1,2, Jun ZHANG1,2, Hao WANG1,2()   

  1. 1.School of Microelectronics,Hubei University,Wuhan 430062,China
    2.Hubei Yangtze Memory Laboratories,Wuhan 430205,China
  • Received:2024-01-29 Accepted:2024-05-15 Published:2024-07-01 Online:2024-08-03
  • Contact: Li TAO,Hao WANG
  • About author:wangh@hubu.edu.cn
    litao@hubu.edu.cn
  • Supported by:
    the Natural Science Foundation of Hubei Province(2022CFB402);the National Natural Science Foundation of China(52272198)

Abstract:

With the development of social industrialization, energy issues have become a hot topic at present. Traditional lithium-ion batteries, due to their poor safety and high cost, cannot meet the current application needs in the energy storage field in the long term. Therefore, the development of suitable new energy has aroused people's deep thinking. Aqueous zinc-ion batteries (AZIBs) have attracted attention from the scientific research community in recent years due to their high safety, cleanliness, and other advantages. However, dendrites are easily grown on the zinc anode, and free water molecules can also corrode the zinc anode, causing side reactions such as hydrogen evolution and passivation, seriously affecting the long-term cycling performance and stability of the battery. This work introduces a new type of ionic liquid additive 1-cyanobutyl-3-methylimidazole chloride (MCBI) to optimize aqueous electrolytes. Before the deposition of zinc ions on the anode surface, MCBI cations will preferentially land on the anode. Due to their special structures of Electron-withdrawing group and nitrogen heterocycles, they will tightly adsorb on the zinc surface in a unique shape of the “Check mark” posture. This provides abundant sites for the deposition of zinc ions, allowing zinc atoms to arrange regularly between MCBI ions, thereby reducing the generation of dendrites. Due to the steric hindrance effect, by-products (Zinc hydroxide sulfate) will also accumulate in an orderly manner around additive ions, forming channels for uniform deposition of zinc ions; The hydrophobic alkyl groups of MCBI cations will repel most of the free water molecules outside the anode, thereby reducing hydrogen evolution reaction (HER). In this work, under the optimal concentration conditions, the Coulomb efficiency of Zn//Cu asymmetric cell with MCBI additive can reach 99.37% after 200 cycles; Zn//Zn symmetric batteries can stably cycle for more than 1600 h at low current density (0.5 mA/cm2), and can cycle for more than 1000 h at 10 mA/cm2, 5 mA·h/cm2. Finally, VO2 as the cathode maintains a high-capacity retention rate of 88.5% after 500 cycles in the full battery. This work provides new ideas for the anode modification strategy of aqueous zinc ion batteries.

Key words: Aqueous zinc ion battery, Electrolyte, Additive, Zinc anode, Dendrite, Ionic liquid

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