Cooperative Solvation‐Interface Engineering via Cell Membrane‐Inspired Hydrated Nanodomains for High‐Mass‐Loading Zinc‐Ion Batteries

Abstract Inspired by the amphiphilic structure of cell membrane phospholipids. Here, a bionic hydrated nanodomains (BHNs) hydrated eutectic electrolyte strategy to realize high‐δ‐MnO 2 ‐loading Zn||MnO 2 batteries with fast kinetics and high Mn utilization is proposed. Specifically, the nano‐confinement effect of BHNs significantly hinders molecular movement and proton delocalization. The amphiphilic structure of sulfoxide (SL) coordinates with Zn 2 ⁺ to form SL‐[Zn(H 2 O) 5 ] 2+ complexes, simultaneously suppressing water activity, inhibiting side reactions, and enhancing electrode wettability. In particular, a dynamically confined cathode interface suppresses Jahn‐Teller distortion in high‐loading δ‐MnO 2 . Accordingly, the symmetrical cell with SL exhibits outstanding stability (5000 h) at the current density of 1.0 mA·cm −2 /1.0 mAh·cm −2 compared to the cell without SL (690 h). Surprisingly, the Zn battery employing a δ‐MnO 2 cathode with high loading (20 mg·cm −2 ) exhibits stable cycling over 5000 cycles. Furthermore, the pouch cell exhibits a high CE of 88% from self‐discharge measurements after 48 h at the fully charged state and sustains 2000 long‐term cycles at 0.5 A·g −1 . This work establishes a fundamental framework for manipulating aqueous electrolytes through hierarchical molecular engineering, offering a generalized design principle for achieving unprecedented stability in rechargeable batteries.