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Herein, we identify anion\u2010dipole binding energy and electrostatic potential difference as double descriptors for screening trace additives as molecular captors for anions, and propose an anion\u2010dipole catalytic decomposition strategy to tailor the SEI. Specifically, electron\u2010deficient aromatic acetophenone preferentially enters the electrical double layer, selectively recognizing and concentrating anions. Concurrently, it catalyzes anion decomposition by accelerating bond\u2010cleavage kinetics and reducing activation free energy, forming the inorganic\u2010rich SEI. This tailored interface yields a high Zn\n                    <jats:sup>2+<\/jats:sup>\n                    transference number (0.75), accelerates desolvation, and promotes planar (002)\u2010textured Zn deposition. Consequently, Zn\/\/Zn symmetric cells exhibit exceptional cycling stability (7200 h), and an Ah\u2010level Zn\/\/VO\n                    <jats:sub>2<\/jats:sub>\n                    pouch cell with cathode mass loading of 20 mg\u00b7cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    delivers a capacity of 4.28 Ah at 0.2 A\u00b7g\n                    <jats:sup>\u22121<\/jats:sup>\n                    and retains 88.9% of its initial capacity after 100 cycles at 1 A\u00b7g\n                    <jats:sup>\u22121<\/jats:sup>\n                    .\n                  <\/jats:p>","DOI":"10.1002\/anie.7075150","type":"journal-article","created":{"date-parts":[[2026,10,9]],"date-time":"2026-10-09T05:06:56Z","timestamp":1791522416000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Anion\u2010Dipole Catalytic Decomposition Enables Robust Solid Electrolyte Interfaces for Ah\u2010Level Aqueous Zinc 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