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Here, a covalent polymer (PCD) is reported as an anode material for aqueous calcium\u2010ion batteries, operating through a Ca\n                    <jats:sup>2+<\/jats:sup>\n                    \/H\n                    <jats:sup>+<\/jats:sup>\n                    storage mechanism associated with redox\u2010active C\u2550N moieties. Proton adsorption dynamically modifies the interfacial microenvironment and induces the reversible formation of a Ca(OH)\n                    <jats:sub>2<\/jats:sub>\n                    surface phase. Rather than impairing performance, this proton\u2010mediated interfacial Ca(OH)\n                    <jats:sub>2<\/jats:sub>\n                    effectively suppresses hydrogen evolution, enabling stable operation at extended negative potentials. As a result, the PCD anode delivers high capacity, rapid charge\u2013discharge response, and exceptional cycling stability. A 43\u2009mAh pouch cell retains 80.4% of its capacity over 1900 cycles (&gt;1000\u2009h), representing a significant step forward in aqueous Ca\n                    <jats:sup>2+<\/jats:sup>\n                    storage. These findings reveal that proton\u2010induced interfacial phases can be harnessed to regulate parasitic reactions, offering a new paradigm for the design of stable aqueous battery electrodes.\n                  <\/jats:p>","DOI":"10.1002\/smll.75574","type":"journal-article","created":{"date-parts":[[2026,9,24]],"date-time":"2026-09-24T08:08:41Z","timestamp":1790237321000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Proton\u2010Mediated Dynamic Interfacial Regulation in a Covalent Polymer Anode for Stable Aqueous Calcium\u2010Ion Batteries"],"prefix":"10.1002","author":[{"given":"Xiangyong","family":"Zhang","sequence":"first","affiliation":[{"name":"Faculty of Materials Science and Energy Engineering Shenzhen University of Advanced Technology  Shenzhen China"},{"name":"Songshan Lake Materials Laboratory  Dongguan Guangdong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chunfang","family":"Wang","sequence":"additional","affiliation":[{"name":"Songshan Lake Materials Laboratory  Dongguan Guangdong China"},{"name":"State Key Laboratory of Powder Metallurgy Central South University  Changsha China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junhao","family":"Zhang","sequence":"additional","affiliation":[{"name":"Faculty of Materials Science and Energy Engineering Shenzhen University of Advanced Technology  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Senlin","family":"Li","sequence":"additional","affiliation":[{"name":"Faculty of Materials Science and Energy Engineering Shenzhen University of Advanced Technology  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Feng","family":"Liu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Powder Metallurgy Central South University  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