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However, unstable Na plating\/stripping and uncontrolled solid electrolyte interphase (SEI) evolution still hinder their practical application. In this work, we investigate the impact of grain\u2010boundary density in the Cu substrate on the performance of AFSBs. The results reveal that higher grain\u2010boundary density Cu exhibits a stronger affinity for sodium and can lower the sodium nucleation energy barriers, facilitating the formation of highly crystalline and densely packed sodium deposits. Moreover, the high surface energy at grain\u2010boundaries strengthens anion adsorption, leading to an anion\u2010rich interfacial solvation structure, which results in the formation of a thin, NaF\u2010rich stable SEI film. Anode\u2010free cells constructed with ultrahigh\u2010grain\u2010boundary density Cu (UGB\u2010Cu) and Na\n                    <jats:sub>3<\/jats:sub>\n                    V\n                    <jats:sub>2<\/jats:sub>\n                    (PO\n                    <jats:sub>4<\/jats:sub>\n                    )\n                    <jats:sub>3<\/jats:sub>\n                    (NVP) cathode achieved stable cycling for 800 cycles at 5C with an average coulombic efficiency (CE) of 99.97%. This work elucidates the dual role of grain\u2010boundary in improving both substrate\u2010sodium affinity and interfacial SEI chemistry, highlighting grain\u2010boundary engineering of Cu foils as a practical and scalable pathway toward high\u2010performance AFSBs.\n                  <\/jats:p>","DOI":"10.1002\/adma.202522541","type":"journal-article","created":{"date-parts":[[2026,1,7]],"date-time":"2026-01-07T05:17:06Z","timestamp":1767763026000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":16,"title":["Grain\u2010Optimized Copper Current Collectors for Highly Stable Anode\u2010Free Sodium Batteries"],"prefix":"10.1002","volume":"38","author":[{"given":"Yujie","family":"Chen","sequence":"first","affiliation":[{"name":"School of Chemical Engineering The University of Adelaide  Adelaide South Australia 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