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Herein, these issues have been addressed through the use of a redox\u2010active salen\u2010based framework polymer (RSFP) containing multiple redox\u2010active centers in \u03c0\u2010conjugated configuration for applications in lithium\u2010ion batteries (LIBs). Based on its unique architecture, RSFP exhibits a superior reversible capacity of 671.8 mAh g<jats:sup>\u22121<\/jats:sup> at 0.05 A g<jats:sup>\u22121<\/jats:sup> after 168 charge\u2010discharge cycles. Importantly, the lithiation\/de\u2010lithiation performance is enhanced during operation, leading to an unprecedented reversible capacity of 946.2 mAh g<jats:sup>\u22121<\/jats:sup> after 3500 cycles at 2 A g<jats:sup>\u22121<\/jats:sup>. The structural evolution of RSFP is studied ex situ using X\u2010ray photoelectron spectroscopy, revealing multiple active C\u2550N, C\u2500O, and C\u2550O sites and aromatic sites such as benzene rings. Remarkably, the emergence of C\u2550O originated from C\u2500O is triggered by an electrochemical process, which is beneficial for improving reversible lithiation\/delithiation behavior. Furthermore, the respective strong and weak binding interactions between redox centers and lithium ions, corresponding to theoretical capacities of 670.1 and 938.2 mAh g<jats:sup>\u22121<\/jats:sup>, have been identified by density functional theory calculations manifesting 14\u2010electron redox reactions. This work sheds new light on routes for the development of redox\u2010active organic materials for energy storage applications.<\/jats:p>","DOI":"10.1002\/smll.202309321","type":"journal-article","created":{"date-parts":[[2024,3,26]],"date-time":"2024-03-26T04:51:01Z","timestamp":1711428661000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["14\u2010Electron Redox Chemistry Enabled by Salen\u2010Based \u03c0\u2010Conjugated Framework Polymer Boosting High\u2010Performance Lithium\u2010Ion Storage"],"prefix":"10.1002","volume":"20","author":[{"given":"Xinlu","family":"Zhang","sequence":"first","affiliation":[{"name":"Shanghai Key Laboratory of Magnetic Resonance School of Physics and Electronic Science East China Normal University  Shanghai 200241 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Seyedeh Alieh","family":"Kazemi","sequence":"additional","affiliation":[{"name":"Centre for Catalysis and Clean Energy School of Environment and Science Gold Coast Campus Griffith University  Southport 4222 Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2286-4307","authenticated-orcid":false,"given":"Xingtao","family":"Xu","sequence":"additional","affiliation":[{"name":"Marine Science and Technology Collage Zhejiang Ocean University  Zhoushan 316022 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jonathan P.","family":"Hill","sequence":"additional","affiliation":[{"name":"Research Center for Materials Nanoarchitectonics (MANA) National Institute for Materials Science (NIMS)  1\u20101 Namiki Tsukuba Ibaraki 305\u20100044 Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiachen","family":"Wang","sequence":"additional","affiliation":[{"name":"Shanghai Key Laboratory of Magnetic Resonance School of Physics and Electronic Science East China Normal University  Shanghai 200241 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haibo","family":"Li","sequence":"additional","affiliation":[{"name":"Ningxia Key Laboratory of Photovoltaic Materials Ningxia University  Yinchuan Ningxia 750021 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Saad M.","family":"Alshehri","sequence":"additional","affiliation":[{"name":"Chemistry Department College of Science King Saud University  P.O. 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