Achieving Highly Reversible and Dendrite‐Free Zinc Anode Using Dual‐Function 1,2‐DACH Electrolyte Additive Via Reconstructed Solvation Structure and In Situ Interfacial Protective Layer

Abstract Metallic zinc anode always suffers from dendritic growth and side reactions induced by active H 2 O in aqueous electrolytes, which severely restrict its practical application in aqueous zinc ion batteries (AZIBs). Herein, cis‐1,2‐cyclohexanediamine (1,2‐DACH) as a novel electrolyte additive is proposed to achieve a dendrite‐free and highly reversible Zn anode. The 1,2‐DACH additive contains two adjacent amino groups, which can not only provide strong coordination with Zn 2+ to reconstruct the solvation structure of Zn 2+ , but also deliver enhanced adsorbability with the Zn anode to induce an in situ interfacial protective layer. Consequently, the Zn anode without side reactions and corrosion but uniform Zn deposition is achieved. Particularly, the Zn anode shows excellent cycling stability (4880 h at 1 mA cm −2 , 1 mAh cm −2 , and 1300 h at 5 mA cm −2 , 5 mAh cm −2 ), and enhanced coulombic efficiency (99.9% upon 2300 cycles at 5 mA cm −2 , 1 mAh cm −2 ). Besides, the assembled Zn||V 2 O 5 full cell can maintain a high capacity retention of 88.7% after 1400 cycles at 1 A g −1 , and cycle more than 3500 cycles at 3 A g −1 . The work may enable the design and deep understanding of dual‐function electrolyte additives for durable AZIBs.