<p>Aqueous zinc-ion batteries (AZIBs) with high theoretical capacity, excellent safety, low cost, and environmental friendliness are promising for next-generation large-scale energy storage. However, their commercial application is hindered by Zn dendrite formation, hydrogen evolution reaction (HER), and Zn corrosion. In this work, sodium cyclamate (SC) is introduced as an electrolyte additive to address these problems. Experimental results demonstrate that this additive inhibits HER and Zn corrosion, and also suppresses the formation of Zn dendrites. Density functional theory calculations reveal that cyclohexylsulfamate ions (C<sup>−</sup>) derived from SC interact more strongly with Zn<sup>2+</sup>, enabling the reconstruction the Zn<sup>2+</sup> solvation structure and the H-bond network, and inhibiting hydrogen evolution and Zn corrosion. Moreover, they also preferentially adsorb on the surface of Zn anode, modifying the electrode–electrolyte interface. The increased nucleation overpotential and three-dimensional diffusion of Zn<sup>2+</sup> facilitate uniform Zn deposition. Thus, cells with Zn foil serving as the anode achieve significantly enhanced performance. The Zn||Zn cells are able to operate continuously for over 700&#xa0;h at 10&#xa0;mA&#xa0;cm<sup>−2</sup> and 5&#xa0;mAh&#xa0;cm<sup>−2</sup>. This work thus offers a simple and effective strategy to stabilize Zn anodes at relatively high current density and large areal capacity, facilitating the development of AZIBs for large-scale energy storage.</p> Graphical Abstract <p></p>

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Solvation and Interface Regulation via Sodium Cyclamate for Stable Zn Anodes

  • Xueyao Mo,
  • Mengjie Zhu,
  • Yan Xu,
  • Xuena Xu,
  • Yidong Miao,
  • Liluo Shi,
  • Xiangjun Kong,
  • Wenchang Zhuang,
  • Ming Song

摘要

Aqueous zinc-ion batteries (AZIBs) with high theoretical capacity, excellent safety, low cost, and environmental friendliness are promising for next-generation large-scale energy storage. However, their commercial application is hindered by Zn dendrite formation, hydrogen evolution reaction (HER), and Zn corrosion. In this work, sodium cyclamate (SC) is introduced as an electrolyte additive to address these problems. Experimental results demonstrate that this additive inhibits HER and Zn corrosion, and also suppresses the formation of Zn dendrites. Density functional theory calculations reveal that cyclohexylsulfamate ions (C) derived from SC interact more strongly with Zn2+, enabling the reconstruction the Zn2+ solvation structure and the H-bond network, and inhibiting hydrogen evolution and Zn corrosion. Moreover, they also preferentially adsorb on the surface of Zn anode, modifying the electrode–electrolyte interface. The increased nucleation overpotential and three-dimensional diffusion of Zn2+ facilitate uniform Zn deposition. Thus, cells with Zn foil serving as the anode achieve significantly enhanced performance. The Zn||Zn cells are able to operate continuously for over 700 h at 10 mA cm−2 and 5 mAh cm−2. This work thus offers a simple and effective strategy to stabilize Zn anodes at relatively high current density and large areal capacity, facilitating the development of AZIBs for large-scale energy storage.

Graphical Abstract