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Pushing intercalation\u2010type cathodes into conversion is certainly desirable, conventionally with great sacrificing cycling\u2010stability, kinetics, and discharge potential. To date, limited progress has been achieved in overcoming this longstanding and formidable performance trade\u2010off. Herein, it is demonstrated that by loosening cation coordination in dilute aqueous systems, typical intercalation\u2010type electrodes (Bi\n                    <jats:sub>2<\/jats:sub>\n                    Se\n                    <jats:sub>3<\/jats:sub>\n                    ) can be unexpectedly extended into the conversion regime, yielding a twofold capacity increase of 417.6 mAh g\n                    <jats:sup>\u22121<\/jats:sup>\n                    with an excellent combination of reversible lifespan (20\u2009000 cycles with a decay rate of 0.013\u2030), rate capability (314.6 mAh g\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 30 A g\n                    <jats:sup>\u22121<\/jats:sup>\n                    ), and enhanced operating potential. Composited\n                    <jats:italic>operando<\/jats:italic>\n                    synchrotron X\u2010ray diffraction technology, first\u2010principal calculations, and ex situ X\u2010ray absorption spectroscopy with electron microscopy analyses indicated that hydrophobic perchlorate optimizes the solvation coordination and charge transfer of cations, which overall decreases the interfacial reaction barrier and enhances the reaction potential, hence initiating unique reversible and depth intercalation\u2012conversion mechanisms. Well\u2010characterized loosening cation coordination further ensures high ion mobility, extraordinary low\u2010temperature performance, and robust operation in quasi\u2010solid\u2010state pouch cells, offering key insights for improving the energy density of aqueous batteries.\n                  <\/jats:p>","DOI":"10.1002\/adma.202507108","type":"journal-article","created":{"date-parts":[[2025,8,30]],"date-time":"2025-08-30T08:33:27Z","timestamp":1756542807000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Breaking the Conversion Limit in an Intercalation\u2010Type Cathode by Loosening Aqueous Cation Coordination"],"prefix":"10.1002","volume":"37","author":[{"given":"Wei","family":"Zhang","sequence":"first","affiliation":[{"name":"Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute Chinese Academy of Sciences  Shanghai 201204 China"},{"name":"Shanghai Institute of Applied Physics 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