Recent efforts to improve zinc metal anode reversibility in aqueous electrolytes have primarily focused on tailoring Zn solvation. We propose a complementary approach to directly engineer the anode interphase with the help of two co-cations. The designed organic co-cations offer distinct improvements: a partially fluorinated pyrrolidinium cation effectively suppresses parasitic reactions such as hydrogen evolution (<6 μA cm), while an ether-functionalized ammonium cation inhibits dendrite formation (almost 10 Ah cm cumulative capacity, >1 year, Zn||Zn). Only 3 wt % of the co-cation combination enables full utilization of a 5-mAh cm reservoir with over 99% Coulombic efficiency and 1,000 cycles with 20% reservoir utilization. We further validate this concept in Zn metal batteries with various cathode chemistries (O, polyaniline, and HNaVO), and we have achieved significant enhancements in performance. This suggests co-cations are a promising and universal approach to improve metal anode reversibility across emerging battery chemistries.

中文翻译：

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设计高度可逆水性锌电池的界面

最近改善水性电解质中锌金属阳极可逆性的努力主要集中在调节锌溶剂化。我们提出了一种补充方法，在两种共阳离子的帮助下直接设计阳极界面。设计的有机共阳离子提供了明显的改进：部分氟化的吡咯烷鎓阳离子有效抑制寄生反应，例如析氢（<6 μA cm），而醚功能化的铵阳离子抑制枝晶形成（几乎10 Ah cm累积容量，>1年，Zn||Zn)。仅 3 wt% 的共阳离子组合即可充分利用 5-mAh cm 储层，库仑效率超过 99%，循环 1,000 次时储层利用率为 20%。我们在具有各种阴极化学物质（O、聚苯胺和 HNaVO）的锌金属电池中进一步验证了这一概念，并且我们在性能方面取得了显着提高。这表明共阳离子是一种有前途且通用的方法，可以提高新兴电池化学物质中金属阳极的可逆性。