Aqueous zinc metal batteries (AZMBs) are limited by water-driven parasitic reactions and unstable Zn deposition. We report a hydrogen-bond-mediated interfacial water-masking strategy using isosorbide dimethyl ether (IDE), a symmetric molecule with electron-rich sites and multiple hydrogen-bond acceptors, to regulate Zn interfacial chemistry at the molecular level. Here, IDE reconstructs the outer hydrogen-bonding network to reduce water activity without occupying the primary Zn2+ solvation sheath. Density-functional analysis further reveals facet-selective adsorption of IDE on Zn(100)/(101), guiding deposition toward the low-energy (002) orientation. IDE-related complexes also promote the formation of an inorganic SEI layer, yielding a compact, low-reactivity interface. With this cooperative regulation, the optimized ZSE–IDE10 electrolyte enables Zn||Zn cells to cycle for over 5400 h at 1 mA cm–2 and 1200 h at 10 mA cm–2, while Zn||NH4V4O10 full cells exhibit improved cycling stability and rate capability. This work establishes a molecular-level design principle for regulating interfacial chemistry in AZMBs.
Chen et al. (Mon,) studied this question.