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To address this issue, axially coordinated Fe single\u2010atom catalysts (Fe\u2010SACs) with asymmetric high\u2010spin N\u2212FeN\n                    <jats:sub>4<\/jats:sub>\n                    sites were synthesized via one\u2010step calcination, enabling selective reactive iron species (RFeS) generation under neutral conditions. In situ x\u2010ray absorption fine structure and the density functional theory analyses revealed that the axial N\u2010coordination stabilizes high\u2010spin states, reduces orbital splitting energy, and enhances\n                    <jats:italic>d<\/jats:italic>\n                    \u2013\n                    <jats:italic>p<\/jats:italic>\n                    hybridization with peroxymonosulfate (PMS), thereby lowering the formation energy of RFeS by 42%. Concurrently, it modulates\n                    <jats:italic>\n                      d\n                      <jats:sub>x<\/jats:sub>\n                      <jats:sup>2<\/jats:sup>\n                      \u2010\n                      <jats:sub>y<\/jats:sub>\n                      <jats:sup>2<\/jats:sup>\n                    <\/jats:italic>\n                    and\n                    <jats:italic>\n                      d\n                      <jats:sub>xy<\/jats:sub>\n                    <\/jats:italic>\n                    orbitals to weaken oxygen binding and promote electron delocalization. This dual modulation achieves &gt; 99% RFeS selectivity, suppressing non\u2010selective radicals. The Fe\u2010SACs\/PMS\/luminol system exhibits 826\u2010fold signal amplification and &lt; 5.8% interferent\u2010induced signal variation, enabling ultrasensitive evaluation of total phenolics (using phenol as a model) in complex water with &lt; 8.3% deviation from high\u2010performance liquid chromatography. This work establishes axial\u2010coordination\u2010directed electronic modulation as a universal design principle for selective catalysis.\n                  <\/jats:p>","DOI":"10.1002\/anie.1246514","type":"journal-article","created":{"date-parts":[[2026,6,7]],"date-time":"2026-06-07T16:24:56Z","timestamp":1780849496000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Axial Coordination Orchestrates Antibonding\u2010State Fermi\u2010Level Proximity and Oxygen Affinity in Single\u2010Atom Iron for Selective Chemiluminescence"],"prefix":"10.1002","volume":"65","author":[{"given":"Peng","family":"Fan","sequence":"first","affiliation":[{"name":"Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute Chinese Academy of Sciences  Shanghai China"},{"name":"Shanghai Engineering Research Center of Biotransformation of Organic Solid Waste School of Ecological and Environmental Sciences East China 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