Multiscale solvation-electronic regulation strategy toward stable Zn anode

The practical advancement of aqueous zinc-ion batteries (AZIBs) is impeded by the intrinsic trade-off between suppressing parasitic hydrogen evolution reaction (HER) and maintaining fast Zn 2+ kinetics. Herein, we propose a synergistic anion-cation regulation strategy to achieve long-cycling AZIBs using Choline Iodide (ChI) as a bifunctional additive. The atomic-level decoupling mechanism is elucidated by synchrotron radiation X-ray absorption spectroscopy (XAS) and density functional theory (DFT). Specifically, ChI acts as an integrated interfacial regulator that facilitates Zn 2+ desolvation, weakens Zn-adsorbate interactions, and promotes the formation of a Zn I inorganic SEI. These coupled effects accelerate Zn plating kinetics while mitigating HER and other parasitic side reactions. Benefiting from this “liquid-solid” dual regulation, the Zn anode exhibits an ultralong lifespan exceeding 11,110 h (>462 days) and over 600 h under 85.47% DOD. Furthermore, full cells coupled with MnO 2 and NH 4 V 4 O 10 cathodes demonstrate outstanding cycling stability, retaining 95.6% (1500 cycles) and 87.5% (1000 cycles) capacity, respectively. Notably, practical pouch cells with a high mass loading of 8.83 mg cm −2 operate stably for over 100 cycles without swelling. This work provides insights into the coupled regulation of interfacial electronic properties and Zn 2+ solvation, offering a feasible strategy for stabilizing AZIBs.