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Herein, a dual\u2010ligand engineering strategy is reported to construct a hierarchical catalyst (CoFe\u2010SA\u2010NP@SNC) featuring atomically dispersed Co\/Fe\u2013N\n                    <jats:sub>4<\/jats:sub>\n                    sites, integrated S\u2010dopants, and confined CoFe alloy nanoparticles within an S,N\u2010codoped carbon framework. A ZIF\u2010mediated dual\u2010template synthesis strategy facilitates the co\u2010construction of multi\u2010scale active centers within the carbon matrix, which form a locally coupled environment beneficial to accelerating oxygen redox kinetics. The optimized CoFe\u2010SA\u2010NP@SNC\u2010700 catalyst exhibits a superior ORR half\u2010wave potential of 0.87 V and a low OER overpotential of 319 mV at 10 mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , yielding a narrow bifunctional potential gap of 0.679 V. Furthermore, the integrated rechargeable Zn\u2010air battery delivers a high peak power density of 179.3 mW cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    and an exceptional lifespan exceeding 400 h. Density functional theory calculations suggest that S dopants and coexisting alloy nanoparticles can jointly regulate the d\u2010band center of Co\/Fe\u2013N\n                    <jats:sub>4<\/jats:sub>\n                    moieties, optimizing the binding affinity of oxygen intermediates and lowering activation barriers for rate\u2010determining steps. This work provides profound insights into coordination\u2010environment engineering for high\u2010performance energy conversion.\n                  <\/jats:p>","DOI":"10.1002\/smll.75513","type":"journal-article","created":{"date-parts":[[2026,9,4]],"date-time":"2026-09-04T03:43:09Z","timestamp":1788493389000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Dual\u2010Ligand Engineering of Atomic Co\/Fe Sites With S\u2010Dopants and CoFe Alloys for Superior Bifunctional Oxygen Electrocatalysis"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0001-8771-860X","authenticated-orcid":false,"given":"Hongtao","family":"Zhou","sequence":"first","affiliation":[{"name":"School of Advanced Manufacturing Guangdong University of Technology  Jieyang China"},{"name":"Guangdong Engineering Technology Research Center of Modern Fine Chemical Engineering School of Chemical Engineering and Light Industry Guangdong 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