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While diatomic catalysts (DACs) have demonstrated superior performance in various catalytic reactions due to their ability to facilitate synergistic charge interactions, their application in AZIBs remains unexplored. Herein, we present, for the first time, a DAC comprising Mn\u2212Zn dual atoms anchored on a nitrogen\u2010doped carbon matrix (MnZn\u2212NC) for iodine loading, resulting in a high\u2010performance AZIB with a capacity of 224\u2005mAh\u2009g\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 1\u2005A\u2009g\n                    <jats:sup>\u22121<\/jats:sup>\n                    and remarkable cycling stability over 320,000\u2005cycles. The electron hopping along the Mn\u2212N\u2212Zn bridge is stimulated via a spin exchange mechanism. This process broadens the Mn 3d\n                    <jats:sub>xy<\/jats:sub>\n                    band width and enhances the metallic character of the catalyst, thus facilitating charge transfer between the catalysts and reaction intermediates. Additionally, the increased electron occupancy within the d\u2010orbital of Zn elevates Zn's d\u2010band center, thereby enhancing chemical interactions between MnZn\u2212NC and I\u2010based species. Furthermore, our mechanism demonstrates potential applicability to other Metal\u2010Zn\u2212NC DACs with spin\u2010polarized atoms. Our work elucidates a clear mechanistic understanding of diatomic catalysts and provides new insights into catalyst design for AZIBs.\n                  <\/jats:p>","DOI":"10.1002\/anie.202410848","type":"journal-article","created":{"date-parts":[[2024,9,13]],"date-time":"2024-09-13T05:20:04Z","timestamp":1726204804000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":96,"title":["Diatomic Catalysts for Aqueous Zinc\u2010Iodine Batteries: Mechanistic Insights and Design Strategies"],"prefix":"10.1002","volume":"63","author":[{"given":"Peng","family":"Hei","sequence":"first","affiliation":[{"name":"Department of Chemistry Northeastern University  3-11, Wenhua Road, Heping district Shenyang 110819 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ya","family":"Sai","sequence":"additional","affiliation":[{"name":"Department of Chemistry Northeastern University  3-11, Wenhua Road, Heping district Shenyang 110819 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenjie","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Chemistry Northeastern University  3-11, Wenhua Road, Heping district Shenyang 110819 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jianming","family":"Meng","sequence":"additional","affiliation":[{"name":"Department of Chemistry Northeastern University  3-11, Wenhua Road, Heping district Shenyang 110819 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yulai","family":"Lin","sequence":"additional","affiliation":[{"name":"Department of Chemistry Northeastern University  3-11, Wenhua Road, Heping district Shenyang 110819 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaoqi","family":"Sun","sequence":"additional","affiliation":[{"name":"Department of Chemistry Northeastern University  3-11, Wenhua Road, Heping district Shenyang 110819 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