Surface Tension‐Derived Electrical Double Layer Modification Enables Practical Zinc‐Ion Pouch Cells

Abstract Interface issues such as parasitic reactions and dendrite growth have long been major obstacles hindering the longevity of aqueous zinc‐ion batteries (AZIBs). The quest for more effective strategies to regulate the highly active interface remains a focal point in AZIBs. Herein, a novel interface‐targeted additive N‐Acetoacetylmorpholine (NHM) is introduced, by lowering the interfacial tension and modifying the electrical double layer, to improve the performance of AZIBs. This reconfiguration results in a H 2 O‐poor inner Helmholtz plane, which suppresses parasitic reactions, accelerates interfacial kinetics, and fosters uniform zinc deposition. Consequently, the zinc anode demonstrates impressive cycling durability, exceeding the 3800 h plating/stripping process and 400 h steady cycle at the high depth of discharge (DOD) of 60%. Zn/NH 4 V 4 O 10 full cell demonstrates superior cycling performance, achieving 80% capacity retention after 1500 cycles. Moreover, the pouch cells with highloading cathodes (13.5 mg cm −2 ) can maintain 70% capacity retention after 300 cycles at 0.5 A g −1 . The pouch cell with a controlled N/P ratio (2.63:1) shows excellent cycling stability with 80% capacity retention after 130 cycles. These findings provide valuable insights into interfacial design and offer promising strategies for enhancing the practicality of AZIBs.