Multidentate coordination chemistry remodeling solvation sheath and interfacial evolution for robust aqueous Zn battery

Abstract Aqueous Zn-ion batteries represent a promising platform for grid-scale energy storage, yet the advancement is constrained by persistent interfacial challenges on dendrite growth and parasitic corrosion. Herein, a novel strategy leveraging the multidentate coordination of Zn2+ and solvent molecules is introduced to synergistically tailor the solvation sheath and modulate the interfacial mass-charge conduction. Reconfiguring the inherent H-bond network and interfacial chemistry effectively suppresses side reactions and ensures uniform Zn deposition. Consequently, a Zn||Zn battery delivers an exceptional cumulative plating capacity of 23.0 Ah·cm–2 and operates steadily for over 4600 h under harsh conditions of 10 mA·cm–2. When coupled with an I2 cathode, the full battery retains excellent durability across 65,000 cycles at 10 A·g–1, with an ultralow capacity decay of 0.0004% per cycle. A practical pouch battery delivers 11.5 mAh and maintains 90.0% capacity after 130 cycles. Multiscale spectroscopy and computations elucidate ligand exchange within the solvation sheath and the synergy with a dynamic interfacial adsorption layer, establishing a green and efficient molecular strategy for stabilizing Zn electrochemistry.