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In this work, we present a cost\u2010effective strategy for preparing catalysts consisting of single\u2010atomic Fe sites and Fe<jats:sub>3<\/jats:sub>C clusters encapsulated in nitrogen\u2010doped carbon layers (FeSA\u2010Fe<jats:sub>3<\/jats:sub>C\/NC). The FeSA\u2010Fe<jats:sub>3<\/jats:sub>C\/NC electrocatalyst demonstrates outstanding ORR performance in alkaline electrolytes, achieving a high half\u2010wave potential (<jats:italic>E<\/jats:italic><jats:sub>1\/2<\/jats:sub>\u00a0=\u00a00.902\u00a0V), 4e<jats:sup>\u2212<\/jats:sup> ORR selectivity, and robust methanol tolerance. The exceptional ORR catalytic performance is credited to the relatively substantial specific surface area and the optimal arrangement of active sites, including atomically dispersed Fe\u2013N sites and synergistic Fe<jats:sub>3<\/jats:sub>C clusters. In situ spectroelectrochemical characterization and theoretical calculations verify that Fe<jats:sub>3<\/jats:sub>C clusters disrupt the symmetric electronic structure of Fe\u2013N<jats:sub>4<\/jats:sub>, optimizing 3d orbitals of Fe centers, thereby accelerating O\u2500O bond cleavage in *OOH to boost ORR activity. Furthermore, a zinc\u2013air battery constructed with FeSA\u2010Fe<jats:sub>3<\/jats:sub>C\/NC demonstrates excellent potential in energy storage application, yielding a maximum power density of 151.3\u00a0mW cm<jats:sup>\u22122<\/jats:sup> and robust cycling durability surpassing that of commercial Pt\/C catalysts. This study establishes a cost\u2010effective route for producing metal\u2010based carbon electrocatalysts with exceptional performance using environmentally friendly raw materials.<\/jats:p>","DOI":"10.1002\/anie.202501266","type":"journal-article","created":{"date-parts":[[2025,3,11]],"date-time":"2025-03-11T08:08:47Z","timestamp":1741680527000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":117,"title":["Synergistic Catalysts with Fe Single Atoms and Fe<sub>3<\/sub>C Clusters for Accelerated Oxygen Adsorption Kinetics in Oxygen Reduction Reaction"],"prefix":"10.1002","volume":"64","author":[{"given":"Chunlian","family":"Liu","sequence":"first","affiliation":[{"name":"Guangdong Engineering Technology Research Center for Sensing Materials Devices Guangzhou Key Laboratory of Sensing Materials Devices School of Chemistry and Chemical Engineering Guangzhou University  Guangzhou 510006 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