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However, understanding the spin\u2010related origin of catalytic activity in heterogeneous molecular electrocatalysts still remains challenging. Herein, a molecular\u2010atomic coupled catalyst is constructed by integrating iron phthalocyanine (FePc) molecules with Fe\u2010N\n                    <jats:sub>4<\/jats:sub>\n                    atomic sites anchored on nitrogen\u2010doped carbon nanotubes (FePc\u2010Fe\u2010NCNT). The strong electronic coupling between FePc and the Fe\u2010N\n                    <jats:sub>4<\/jats:sub>\n                    \u2010containing carbon substrate triggers a transition of the Fe sites from a low\u2010spin state to an intermediate\u2010spin state. Additionally, the formation of \u03c3* bonds between the electron\u2010injected perpendicular d\n                    <jats:sub>z2<\/jats:sub>\n                    orbitals of intermediate\u2010spin Fe and the 2p orbitals of adsorbed oxygen species suppresses site blocking and accelerates OH* desorption, thereby enhancing the reaction kinetics of the oxygen reduction reaction (ORR). The resulting catalyst exhibits exceptional ORR activity in alkaline media, reaching a half\u2010wave potential of 0.89 V and negligible degradation after 10,000 cycles. Remarkably, the quasi\u2010solid\u2010state Zinc\u2010air battery based on this prepared catalyst operates stably from \u221240 to 70\u00a0\u00b0C with minimal performance loss. This work reveals a spin\u2010state manipulation strategy for the development of advanced molecular catalysts and provides new insights into the regulation of electronic structure for energy conversion technologies.\n                  <\/jats:p>","DOI":"10.1002\/advs.202510306","type":"journal-article","created":{"date-parts":[[2025,7,18]],"date-time":"2025-07-18T11:18:52Z","timestamp":1752837532000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":19,"title":["Spin\u2010State Engineering of Iron Phthalocyanine D\u2010Orbitals via Atomic Fe\u2010N\n                    <sub>4<\/sub>\n                    Coupling for Enhanced Oxygen Reduction Reaction"],"prefix":"10.1002","volume":"12","author":[{"given":"Ze","family":"Lv","sequence":"first","affiliation":[{"name":"National Engineering Research Center for Dyeing and Finishing of Textiles College of Chemistry and Chemical Engineering Donghua University  No.2999 North Renmin Road Shanghai 201620 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zheng","family":"Shu","sequence":"additional","affiliation":[{"name":"Joint Key Laboratory of the Ministry of Education Institute of Applied Physics and Materials Engineering University of Macau  Macao SAR 999078 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yang","family":"Qiu","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering Sichuan University  Chengdu 610065 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiawei","family":"Luo","sequence":"additional","affiliation":[{"name":"National Engineering Research Center for Dyeing and Finishing of Textiles College of Chemistry and Chemical Engineering Donghua University  No.2999 North Renmin Road Shanghai 201620 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kaibing","family":"Xu","sequence":"additional","affiliation":[{"name":"State Key Laboratory for 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