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These reactions driven by unsaturated vanadium sites and solvent enrichment cause rapid capacity fade. Herein, we propose a molecular interfacial engineering strategy using rationally designed organic phosphate additives. These additives stabilize vanadium via\n                    <jats:italic>\u03c0\u2010d<\/jats:italic>\n                    orbital hybridization and regulate the interfacial microenvironment through three\u2010dimensional steric shielding, passivating reactive species, and suppressing solvent enrichment. Guided by a descriptor\u2010driven screening process (Mulliken charge, van der Waals volume, O\n                    <jats:italic>2p<\/jats:italic>\n                    band center, \u0394\n                    <jats:italic>E<\/jats:italic>\n                    (O\n                    <jats:italic>2p<\/jats:italic>\n                    band center\u2010V\n                    <jats:italic>3d<\/jats:italic>\n                    band center)), tris(trimethylsilyl) phosphate (TMSP) is identified as the optimal electrolyte modifier. The TMSP\u2010tailored electrolyte promotes in situ formation of a thin, compact, and inorganic\u2010rich interphase on both the NVPF cathode and the hard carbon (HC) anode, effectively mitigating vanadium species dissolution and parasitic side reactions. Consequently, the 4.3\u00a0V NVPF||HC pouch cell can deliver exceptional cycling stability, retaining 85.24% of its capacity after 1500 cycles (416.7 days) at 0.3 C, and achieve a high energy density of 161\u00a0Wh kg\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    . This work establishes a design principle that couples orbital hybridization with steric shielding to construct ultra\u2010stable interfaces in high\u2010voltage battery systems.\n                  <\/jats:p>","DOI":"10.1002\/anie.6618249","type":"journal-article","created":{"date-parts":[[2026,4,2]],"date-time":"2026-04-02T08:22:05Z","timestamp":1775118125000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":9,"title":["Synergistic Orbital Hybridization and Steric Shielding for Stabilizing High\u2010Voltage Interfaces in 4.3\u00a0V Sodium\u2010Ion Batteries"],"prefix":"10.1002","volume":"65","author":[{"given":"Bin","family":"Ye","sequence":"first","affiliation":[{"name":"Hefei National Research Center for Physical Sciences at the Microscale, Department of Materials Science and Engineering University of Science and Technology of China  Hefei Anhui 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