Anion-Dipole Catalytic Decomposition Enables Robust Solid Electrolyte Interfaces for Ah-Level Aqueous Zinc Batteries.

Constructing robust inorganic-rich solid electrolyte interfaces (SEIs) without the compromised safety and interfacial kinetics remains challenging for aqueous zinc ion batteries. Herein, we identify anion-dipole binding energy and electrostatic potential difference as double descriptors for screening trace additives as molecular captors for anions, and propose an anion-dipole catalytic decomposition strategy to tailor the SEI. Specifically, electron-deficient aromatic acetophenone preferentially enters the electrical double layer, selectively recognizing and concentrating anions. Concurrently, it catalyzes anion decomposition by accelerating bond-cleavage kinetics and reducing activation free energy, forming the inorganic-rich SEI. This tailored interface yields a high Zn2+ transference number (0.75), accelerates desolvation, and promotes planar (002)-textured Zn deposition. Consequently, Zn//Zn symmetric cells exhibit exceptional cycling stability (7200 h), and an Ah-level Zn//VO2 pouch cell with cathode mass loading of 20 mg·cm-2 delivers a capacity of 4.28 Ah at 0.2 A·g-1 and retains 88.9% of its initial capacity after 100 cycles at 1 A·g-1.