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Here, we report an axial chlorine (Cl) spin\u2010collar on Mn single\u2010atom sites (MnNC\u2010Cl), which tunes Mn\n                    <jats:sup>II<\/jats:sup>\n                    from medium spin (MS,\n                    <jats:italic>S<\/jats:italic>\n                    \u00a0=\u00a03\/2, d\n                    <jats:sub>yz<\/jats:sub>\n                    <jats:sup>2<\/jats:sup>\n                    , d\n                    <jats:sub>xy<\/jats:sub>\n                    <jats:sup>1<\/jats:sup>\n                    , d\n                    <jats:sub>xz<\/jats:sub>\n                    <jats:sup>1<\/jats:sup>\n                    , d\n                    <jats:sub>z2<\/jats:sub>\n                    <jats:sup>1<\/jats:sup>\n                    , d\n                    <jats:sub>x2\u2212y2<\/jats:sub>\n                    <jats:sup>0<\/jats:sup>\n                    ) to low spin (LS,\n                    <jats:italic>S<\/jats:italic>\n                    \u00a0=\u00a01\/2, d\n                    <jats:sub>yz<\/jats:sub>\n                    <jats:sup>2<\/jats:sup>\n                    , d\n                    <jats:sub>xy<\/jats:sub>\n                    <jats:sup>2<\/jats:sup>\n                    , d\n                    <jats:sub>xz<\/jats:sub>\n                    <jats:sup>1<\/jats:sup>\n                    , d\n                    <jats:sub>z2<\/jats:sub>\n                    <jats:sup>0<\/jats:sup>\n                    , d\n                    <jats:sub>x2\u2212y2<\/jats:sub>\n                    <jats:sup>0<\/jats:sup>\n                    ). This spin transition lowers the Mn\u2500*OH bond order from 1.5 to 1, weakening *OH over\u2010adsorption and steering the reaction toward an efficient four\u2010electron (4e\n                    <jats:sup>\u2212<\/jats:sup>\n                    ) pathway. The MnNC\u2010Cl catalyst delivers a high half\u2010wave potential (E\n                    <jats:sub>1\/2<\/jats:sub>\n                    ) of 0.829\u00a0V in acid, with a 2.7\u00d7 higher turnover frequency (TOF@0.85\u00a0V) and 1.2 \u00d7 greater peak power density in H\n                    <jats:sub>2<\/jats:sub>\n                    \u2010air fuel cells than the pristine counterpart. Through theoretical and experimental investigations, the mechanism of the axial Cl spin\u2010collar is elucidated: symmetry\u2010breaking crystal field distortion induced by axial Cl triggers electron transfer from the spin\u2010up d\n                    <jats:sub>z2<\/jats:sub>\n                    to the spin\u2010down d\n                    <jats:sub>xy<\/jats:sub>\n                    orbital, locking Mn into a low\u2010spin state and enhancing catalytic activity. This study establishes a spin\u2010collar strategy for precise regulation of the spin state in Mn centers.\n                  <\/jats:p>","DOI":"10.1002\/anie.2102563","type":"journal-article","created":{"date-parts":[[2026,7,30]],"date-time":"2026-07-30T16:15:13Z","timestamp":1785428113000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["An Axial Chlorine Spin\u2010Collar on Atomic Mn Centers for Oxygen Reduction"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0001-9394-9498","authenticated-orcid":false,"given":"Wu","family":"Wang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical Engineering Xiamen University  Xiamen P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hong\u2010Guan","family":"Li","sequence":"additional","affiliation":[{"name":"School of Metallurgy Northeastern University  Shenyang P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Min\u2010Le","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical Engineering Xiamen University  Xiamen P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huan","family":"Huang","sequence":"additional","affiliation":[{"name":"Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences  Beijing P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jian","family":"Yang","sequence":"additional","affiliation":[{"name":"Center of Advanced Electrochemical Energy Institute of Advanced Interdisciplinary Studies College of Chemistry and Chemical Engineering Chongqing University  Chongqing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jing","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Metastable Materials Science and Technology, Key Laboratory of Heavy Metal Deep\u2010Remediation in Water and Resource Reuse Yanshan University  Qinhuangdao P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rui","family":"Huang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical Engineering Xiamen University  Xiamen P. R. 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