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Here, we propose a thermodynamics\u2010guided screening paradigm, in which the theoretical redox potentials are derived and calculated from the Nernst equation and Gibbs free energy (\u0394\n                    <jats:italic>G<\/jats:italic>\n                    ), thereby effectively predicting and screening cathodes with high working voltage. Based on this, we synthesize Co\n                    <jats:sub>3<\/jats:sub>\n                    (PO\n                    <jats:sub>4<\/jats:sub>\n                    )\n                    <jats:sub>2<\/jats:sub>\n                    with a distinct crystal structure, which is further employed as a model cathode to validate the feasibility of the abovementioned theoretical screening strategy. Electrochemical tests demonstrate that the Al||Co\n                    <jats:sub>3<\/jats:sub>\n                    (PO\n                    <jats:sub>4<\/jats:sub>\n                    )\n                    <jats:sub>2<\/jats:sub>\n                    cell operates at a range of 1.20\u20131.50\u00a0V with a specific capacity of 198.01 mAh g\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    and an ultra\u2010high energy density of 247.4\u00a0Wh kg\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    , which is in excellent agreement with the thermodynamic predictions. Importantly, the cell could stably cycle for over 14\u00a0500 cycles with almost negligible capacity decay. Mechanistic analyses indicate that redox mechanism mainly involves Al\n                    <jats:sup>3+<\/jats:sup>\n                    adsorption\/desorption and shallow intercalation\/de\u2010intercalation processes. On balance, this simple and universal strategy offers an insightful idea for enhancing the working voltage of cathodes, while providing clear design guidelines for the development of high\u2010energy\u2010density energy storage systems.\n                  <\/jats:p>","DOI":"10.1002\/adma.74803","type":"journal-article","created":{"date-parts":[[2026,8,26]],"date-time":"2026-08-26T05:32:11Z","timestamp":1787722331000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Thermodynamics\u2010Guided Screening and Mechanistic Insights for Advanced Cathodes Toward High\u2010Energy\u2010Density Rechargeable Aluminum Batteries"],"prefix":"10.1002","volume":"38","author":[{"given":"Huaizhi","family":"Wang","sequence":"first","affiliation":[{"name":"Beijing Key Laboratory of Environmental Science and Engineering School of Materials Science and Engineering Beijing Institute of Technology  Beijing 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