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While accommodating chloroaluminate ions (AlCl<jats:sub>4<\/jats:sub><jats:sup>\u2212<\/jats:sup>, AlCl<jats:sup>2+<\/jats:sup>, etc.) in redox\u2010active organic compounds offers a promising solution for RABs, the issues of dissolution and low ionic\/electronic conductivities plague the development of organic cathodes. Herein, electron donors are synthetically connected with acceptors to create crosslinked, bipolar\u2010conjugated polymer cathodes. These cathodes exhibit overlapped redox potential ranges for both donors and acceptors in highly concentrated AlCl<jats:sub>3<\/jats:sub>\u2010based ionic liquid electrolytes. This approach strategically enables on\u2010site doping of the polymer backbones during redox reactions involving both donor and acceptor units, thereby enhancing the electron\/ion transfer kinetics within the resultant polymer cathodes. Based on the optimal donor\/acceptor combination, the bipolar polymer cathodes can deliver a high specific capacity of 205\u00a0mAh\u00a0g<jats:sup>\u22121<\/jats:sup> by leveraging the co\u2010storage of AlCl<jats:sub>4<\/jats:sub><jats:sup>\u2212<\/jats:sup> and AlCl<jats:sup>2+<\/jats:sup>. The electrodes exhibit excellent rate performance, a stable cycle life of 60\u00a0000 cycles, and function efficiently at high mass loadings, i.e., 100\u00a0mg cm<jats:sup>\u22122<\/jats:sup>, and at low temperatures, i.e., \u221230\u00a0\u00b0C. The findings exemplify the exploration of high\u2010performing conjugated polymer cathodes for RABs through rational structural design.<\/jats:p>","DOI":"10.1002\/adma.202406106","type":"journal-article","created":{"date-parts":[[2024,8,7]],"date-time":"2024-08-07T01:59:26Z","timestamp":1722995966000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":45,"title":["Regulating the Double\u2010Way Traffic of Cations and Anions in Ambipolar Polymer Cathodes for High\u2010Performing Aluminum Dual\u2010Ion Batteries"],"prefix":"10.1002","volume":"36","author":[{"given":"Lian\u2010Wei","family":"Luo","sequence":"first","affiliation":[{"name":"School of Materials Science and Engineering Shaanxi Normal University  Xi'an 710062 P. R. 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