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Herein, we predicted and screened a bilayer graphite carbon-supported Ir-N\n                    <jats:sub>4<\/jats:sub>\n                    \/Fe-N\n                    <jats:sub>4<\/jats:sub>\n                    catalyst with high ORR activity using density functional theory calculations. Subsequently, various bimetallic single atom supported on 3D ordered macroporous carbon were rationally designed and experimentally synthesized via a colloidal microsphere template-confined reaction method. As anticipated, the resulting Ir-N\n                    <jats:sub>4<\/jats:sub>\n                    \/Fe-N\n                    <jats:sub>4<\/jats:sub>\n                    bimetallic single-atom catalysts (IrFe-SACs) exhibit superior ORR activity and durability, reaching a half-wave potential of 0.928\u00a0V. The IrFe-SACs also demonstrate outstanding performance in Zn-air batteries, including a high discharge power density (314\u00a0mW cm\u207b\n                    <jats:sup>2<\/jats:sup>\n                    ) and excellent cycling stability (~\u20091650 cycles over 550\u00a0h). Further experimental characterizations and theoretical analysis reveal that introducing interlayer-adjacent Ir-N\n                    <jats:sub>4<\/jats:sub>\n                    sites facilitates the transition of Fe-N\n                    <jats:sub>4<\/jats:sub>\n                    from a low-spin state to a medium-spin state, which optimizes the spin polarization of Fe 3d orbitals and enhances the non-localization of the Fe\u2013O\/OH molecular orbital, thereby significantly improving the ORR intrinsic activity and durability of atomic Fe-N\n                    <jats:sub>4<\/jats:sub>\n                    sites.\n                  <\/jats:p>","DOI":"10.1007\/s40820-026-02108-9","type":"journal-article","created":{"date-parts":[[2026,3,5]],"date-time":"2026-03-05T06:51:44Z","timestamp":1772693504000},"update-policy":"https:\/\/doi.org\/10.1007\/springer_crossmark_policy","source":"Crossref","is-referenced-by-count":10,"title":["Modulation of the Spin State of Atomic Fe-N4 Sites with Interlayer-Adjacent Ir-N4 for Superior ORR Activity"],"prefix":"10.1007","volume":"18","author":[{"given":"Yan","family":"Tan","sequence":"first","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Aoshuang","family":"Li","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yijie","family":"Wang","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiucai","family":"Jiang","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yiwen","family":"Cheng","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dongliang","family":"Chao","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuzhong","family":"Zhang","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chuanwei","family":"Cheng","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"297","published-online":{"date-parts":[[2026,3,5]]},"reference":[{"issue":"3","key":"2108_CR1","doi-asserted-by":"publisher","first-page":"2102688","DOI":"10.1002\/aenm.202102688","volume":"12","author":"X Xie","year":"2022","unstructured":"X. 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