<p>The uncontrollable Zn dendrites and serious parasitic side reactions of the zinc anode severely impede the practical application of aqueous zinc-ion batteries. In this work, a unique strategy of multipoint solvate coordination center is proposed, which anchors Zn<sup>2+</sup> and H<sub>2</sub>O with complex sites to establish an intermolecular connection within the asymmetric solvation structure. A hydrated deep eutectic electrolyte based on multi-site methylurea (MU) with Janus properties is developed, in which Zn<sup>2+</sup> and H<sub>2</sub>O interact with MU through Lewis acid-base and hydrogen bonding interaction, and the regulated asymmetric solvation configuration can guide the (002)-ordered Zn deposition. Simultaneously, a small amount of polyethylene glycol (PEG, <i>M</i><sub>w</sub>=20000) can facilitate homogenous (002) Zn deposition by suppressing Zn<sup>2+</sup> transfer kinetics. Benefiting from the rationally regulated solvation structure and PEG molecules adsorbed onto Zn anodes, the side reactions and Zn dendrites are significantly inhibited. As a result, the Zn∥Zn symmetric cell delivers outstanding cycling performance over 3900 h (1 mA cm<sup>−2</sup>, 0.5 mA h cm<sup>−2</sup>). In addition, the Zn∥V<sub>2</sub>O<sub>5</sub> battery maintains 79.2% capacity retention after 1000 cycles at 1 A g<sup>−1</sup>. The results suggest a promising oriented regulation strategy for sustainable aqueous zinc-ion batteries.</p>

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Solvation regulation with Janus solvates for sustainable aqueous Zn ion batteries

  • Ping Jiang,
  • Jianchun Chen,
  • Kean Chen,
  • Weiping Xie,
  • Liangdong Lin,
  • Yongjin Fang,
  • Yonggao Xia,
  • Zhong-Shuai Wu,
  • Zhongxue Chen,
  • Dianbo Ruan,
  • Yuliang Cao

摘要

The uncontrollable Zn dendrites and serious parasitic side reactions of the zinc anode severely impede the practical application of aqueous zinc-ion batteries. In this work, a unique strategy of multipoint solvate coordination center is proposed, which anchors Zn2+ and H2O with complex sites to establish an intermolecular connection within the asymmetric solvation structure. A hydrated deep eutectic electrolyte based on multi-site methylurea (MU) with Janus properties is developed, in which Zn2+ and H2O interact with MU through Lewis acid-base and hydrogen bonding interaction, and the regulated asymmetric solvation configuration can guide the (002)-ordered Zn deposition. Simultaneously, a small amount of polyethylene glycol (PEG, Mw=20000) can facilitate homogenous (002) Zn deposition by suppressing Zn2+ transfer kinetics. Benefiting from the rationally regulated solvation structure and PEG molecules adsorbed onto Zn anodes, the side reactions and Zn dendrites are significantly inhibited. As a result, the Zn∥Zn symmetric cell delivers outstanding cycling performance over 3900 h (1 mA cm−2, 0.5 mA h cm−2). In addition, the Zn∥V2O5 battery maintains 79.2% capacity retention after 1000 cycles at 1 A g−1. The results suggest a promising oriented regulation strategy for sustainable aqueous zinc-ion batteries.