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Herein, by employing a simple n\u2010type azabenzene compound, hexaazatrinaphthalene (HATN), as a template, we introduce strong electron\u2010withdrawing cyano (C\u2261N) groups to drastically reduce its surface electron density, constructing an electron\u2010deficient system with a positive surface potential and a highly positive permanent quadrupole moment (\n                    <jats:italic>Q<\/jats:italic>\n                    <jats:sub>zz<\/jats:sub>\n                    ), denoted as HCNAP. This unique electronic structure triggers anion\u2010\u03c0 interactions and consequently enables anion adsorption. Meanwhile, the C\u2550N and C\u2261N groups on the HCNAP skeleton maintain the function of cation adsorption. As a proof of concept, the symmetric CDI device fabricated with HCNAP exhibits outstanding desalination performance in a 500\u00a0mg L\n                    <jats:sup>\u22121<\/jats:sup>\n                    NaCl solution, achieving a salt adsorption capacity of 53.88\u00a0mg g\n                    <jats:sup>\u22121<\/jats:sup>\n                    and a removal rate of 10.1\u00a0mg g\n                    <jats:sup>\u22121<\/jats:sup>\n                    min\n                    <jats:sup>\u22121<\/jats:sup>\n                    . Theoretical calculations and experimental results clearly reveal the adsorption mechanism of Na\n                    <jats:sup>+<\/jats:sup>\n                    and Cl\n                    <jats:sup>\u2212<\/jats:sup>\n                    . Besides, HCNAP presents favorable adsorption toward three additional cations and anions. This innovative strategy establishes a new paradigm for constructing bifunctional Faradaic electrodes for highly efficient desalination.\n                  <\/jats:p>","DOI":"10.1002\/anie.9286865","type":"journal-article","created":{"date-parts":[[2026,5,21]],"date-time":"2026-05-21T12:47:31Z","timestamp":1779367651000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Cyano\u2010Triggered Strong Anion\u2010\u03c0 Interactions: Unlocking Anion\u2013Cation Adsorption Bifunction"],"prefix":"10.1002","volume":"65","author":[{"given":"Li","family":"Dong","sequence":"first","affiliation":[{"name":"College of Materials and Chemical Engineering Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials China Three Gorges University Yichang China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuang","family":"Li","sequence":"additional","affiliation":[{"name":"College of Materials 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