Lipid Analogues Enhance the Lifespans of Reversible Zn‐Based Aqueous Batteries via Optimal Interfacial Assembly

Abstract The formation of dendrites associated with corrosion reactions undermines the cycling stability of aqueous zinc‐ion batteries (AZBs). Despite extensive efforts, conventional strategies, e.g., electrolyte modification, and artificial protection layers, often suffer from low stability. Inspired by cell membranes, a series of phospholipid analogues C n P m C is designed which can spontaneously adsorb onto the Zn electrode to form a bimolecular protective layer. By tuning the head length or the tail length of the lipid analogues, the nanostructures of the lipid layer can be modified in terms of coverage and thickness, affecting the electrochemical behavior of the electrode. The most optimal electrochemical behavior is found for the adsorption of C 12 P 2 C at a concentration of 1 mM. The bilayer formed by C 12 P 2 C is denser and more stable than those formed by other lipid analogues. The lipid bilayer facilitated the balance of Zn plating/striping, thereby effectively limiting the growth of dendrites and side reactions, further enhancing the reversibility of zinc‐based aqueous batteries. In symmetric battery experiments, C 12 P 2 C can exceed 3600 h under 1 mA cm −2 and 1 mAh cm −2 test conditions. Thus, this study not only demonstrates a bio‐friendly electrode protective material but also provides constructive suggestions on the molecular design of electrode protection material.