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Among\u00a0various electrode materials, vanadium\/iron\u2010based polyanionic compounds show significant potential as SIB cathodes due to their stable structures and high operating voltages, yet challenges persist in electron\/Na\n                    <jats:sup>+<\/jats:sup>\n                    transport and energy density. Although doping is an effective solution, the structure\u2010activity relationship between dopant\u2010induced configuration of octahedral\/tetrahedral units and electrochemical performance remains poorly understood. Herein, the effects of composition and connection type of octahedral and tetrahedral constitutional units on Na\u2010storage properties are systematically re\u2010evaluated. By establishing descriptors and systematic analysis, the regulatory roles of octahedral\/tetrahedral units are elucidated, establishing a fresh research perspective to describe the intrinsic impact of doping types on the structure\u2010activity relationship. Additionally, other modification strategies are discussed to complement the research on the constitutional unit. In industrial applications, balancing electrochemical performance with air stability, cost, and large\u2010scale production remains challenging, creating novel configuration compositions, controlling the structural arrangement of constitutional units, combined with interface and microstructural adjustments, are proposed to achieve multiscale modifications. Simultaneously, theoretical simulations will be employed to predict\/validate their efficacy, providing insights for the rational design of high\u2010performance and low\u2010cost polyanionic compounds for sustainable SIBs.\n                  <\/jats:p>","DOI":"10.1002\/adma.202509966","type":"journal-article","created":{"date-parts":[[2025,8,14]],"date-time":"2025-08-14T13:30:47Z","timestamp":1755178247000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":31,"title":["Controllable Configuration of Constitutional Units in Vanadium\/Iron\u2010Based Polyanionic Compounds for Sodium\u2010Ion Storage"],"prefix":"10.1002","volume":"37","author":[{"ORCID":"https:\/\/orcid.org\/0009-0000-6201-5820","authenticated-orcid":false,"given":"Bochao","family":"Chen","sequence":"first","affiliation":[{"name":"State Key Laboratory of Advanced Chemical Power Sources, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Academy of Advanced Interdisciplinary Studies, College of Chemistry Nankai University  Tianjin 300071 P. 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