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Here, we show that atomically defined iron\u2010oxo clusters can serve as structure\u2010encoded precursors to generate supported Fe ensembles on N\u2010doped carbon (NC), enabling systematic construction of active sites spanning isolated atoms to size\u2010defined multinuclear clusters. During ligand removal and interfacial reconstruction, the molecular structural information is selectively inherited, giving rise to correlated evolution of Fe valence, Fe\u2500Fe coordination and distance, and Fe\u2500N anchoring interactions. Using hydrazine\u2010mediated nitroarene reduction as a model multielectron reaction, we uncover a pronounced nuclearity\u2010dependent transition in the reaction pathway, with optimal activity at intermediate nuclearity (Fe\n                    <jats:sub>6<\/jats:sub>\n                    \u2500NC), attributable to precursor\u2010dependent Fe\u2500Fe cooperation and Fe\u2500N interfacial coupling that stabilize surface hydride species. These findings provide a general basis for translating metal\u2500oxo clusters into functional heterogeneous catalysts.\n                  <\/jats:p>","DOI":"10.1002\/anie.4755364","type":"journal-article","created":{"date-parts":[[2026,9,29]],"date-time":"2026-09-29T11:02:12Z","timestamp":1790679732000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Programming Iron Nuclearity and Coordination for Hydride\u2010Mediated Nitroarene Reduction"],"prefix":"10.1002","author":[{"given":"Jianfei","family":"Yao","sequence":"first","affiliation":[{"name":"Key Lab for Colloid and Interface Science of Ministry of Education, School of Chemistry and Chemical Engineering Shandong University  Jinan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dexin","family":"Wang","sequence":"additional","affiliation":[{"name":"Key Lab for Colloid and Interface Science of Ministry of Education, School of Chemistry and 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