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Atomically dispersed FeN\n                    <jats:sub>4<\/jats:sub>\n                    catalysts are widely regarded as promising platinum\u2010free alternatives for the oxygen reduction reaction (ORR). To overcome the fundamental constraint, we strategically introduce axial N\u2010coordination to the Fe center by employing phenethylamine as a Lewis\u2010base ligand, while using\n                    <jats:italic>\u03c0\u2013\u03c0<\/jats:italic>\n                    stacking between imidazole and a benzene ring to precisely control coordination geometry and prevent sixth\u2010ligand binding. The introduction of an axial ligand markedly enhances the spin polarization of the Fe center and reconfigures its electronic properties by modulating the local ligand field, which promotes more favorable spin\/orbital interactions with oxygen species and fine\u2010tunes the adsorption of reaction intermediates. Through precise spin\u2010electronic tuning, N\u2010FeN\n                    <jats:sub>4<\/jats:sub>\n                    C with an ultralow Fe loading of 0.477% delivers outstanding ORR performance, with a half\u2010wave potential (E\n                    <jats:sub>1\/2<\/jats:sub>\n                    ) of 0.92\u00a0V and a Tafel slope of 57.83\u00a0mV dec\n                    <jats:sup>\u22121<\/jats:sup>\n                    , which corresponds to a 151% improvement in turnover frequency (TOF). This work introduces a rational ligand\u2010field strategy to break the symmetry of single\u2010atom Fe sites, thereby advancing the creation of high\u2010performance, noble\u2010metal\u2010free electrocatalysts.\n                  <\/jats:p>","DOI":"10.1002\/smll.74905","type":"journal-article","created":{"date-parts":[[2026,7,28]],"date-time":"2026-07-28T09:06:02Z","timestamp":1785229562000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Spin\u2010State Modulation of FeN\n                    <sub>4<\/sub>\n                    via Pre\u2010Coordination Axial N\u2010Ligand for Efficient Oxygen Reduction Electrocatalysis"],"prefix":"10.1002","volume":"22","author":[{"given":"Zeyu","family":"Gao","sequence":"first","affiliation":[{"name":"Institute For Carbon Neutrality University of Science and Technology Beijing  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yucheng","family":"Lv","sequence":"additional","affiliation":[{"name":"Institute For Carbon Neutrality University of Science and Technology Beijing  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Linlin","family":"Zhou","sequence":"additional","affiliation":[{"name":"Institute For Carbon Neutrality University of Science and Technology Beijing  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yao","family":"Di","sequence":"additional","affiliation":[{"name":"Institute For Carbon Neutrality University of Science and Technology Beijing  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7312-7131","authenticated-orcid":false,"given":"Zhi","family":"Fang","sequence":"additional","affiliation":[{"name":"School of Materials Shenzhen Campus of Sun Yat\u2010Sen University  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinmei","family":"Hou","sequence":"additional","affiliation":[{"name":"Institute For Carbon Neutrality University of Science and Technology Beijing  Beijing 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