The electrochemical instability of zinc anode caused by surface side reactions and irregular zinc deposition severely hinders the practical application of aqueous zinc ion batteries (AZIBs). In this work, diethylenetriaminepentaacetic acid, pentasodium salt (DTPA) was used as a novel electrolyte additive to modulate the electrochemical stability of Zn anode. The DTPA anion can strongly coordinate with Zn2+, thus enabling the formation of a unique large-size anion-enhanced solvation structure of electrolyte. In this, not only the generation of by-products on Zn anode can be effectively inhibited, but more importantly, the deposition kinetics of Zn2+ can be well regulated to induce even and stable zinc deposition. In addition, DTPA is more prone to chemically adsorbed on the surface of Zn anode than H2O, contributing to the resistance of electrochemical corrosion. Synergistically, the Zn anode demonstrates excellent cycling stability (3850 h at 1 mA cm−2, 1 mAh cm−2, and 500 h at 10 mA cm−2, 10 mAh cm−2), enhanced coulombic efficiency (99.83% upon 3500 cycles at 5 mA cm−2, 1 mAh cm−2), and high reversibility of 1050 h even at a stringent discharge depth of 80%. Particularly, the full cell assembled with NaV3O8·1·5H2O (NaVO) cathode can also operate stably for 1800 cycles at 2 A g−1 with a high capacity retain of 90.8%. This work may pave a new route to achieve high-performance AZIBs by regulating the deposition process of Zn2+ based on large-size anion-enhanced solvation structure of electrolyte.

中文翻译：

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通过大尺寸阴离子增强溶剂化结构实现无枝晶锌沉积，用于高度可逆的锌负极


表面副反应和不规则的锌沉积引起的锌负极电化学不稳定性严重阻碍了水系锌离子电池 （AZIBs） 的实际应用。在本工作中，二乙烯三胺五乙酸五钠盐 （DTPA） 被用作一种新型电解质添加剂，以调节 Zn 负极的电化学稳定性。DTPA 阴离子可以与 Zn2+ 强配位，从而能够形成电解质独特的大尺寸阴离子增强溶剂化结构。这样，不仅可以有效抑制 Zn 负极上副产物的产生，更重要的是可以很好地调节 Zn2+ 的沉积动力学，诱导均匀稳定的锌沉积。此外，DTPA 比 H2O 更容易化学吸附在 Zn 负极表面，有助于抵抗电化学腐蚀。协同作用，锌负极表现出优异的循环稳定性（在 1 mA cm-2 1 mAh cm-2 下 3850 小时，在 10 mA cm-2 10 mAh cm-2 下 500 小时），增强的库仑效率（在 5 mA cm-2 1 mAh cm-2 下循环 3500 次后 99.83%），即使在 80% 的严格放电深度下，也能保持 1050 小时的高可逆性。特别是，用 NaV3O8·1·5H2O （NaVO） 阴极组装的全电池也可以在 2 A g-1 下稳定运行 1800 次循环，容量保持率高达 90.8%。这项工作可能通过基于电解质大尺寸阴离子增强溶剂化结构的 Zn2+ 沉积过程，为实现高性能 AZIBs 铺平了一条新途径。