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However, multi\u2010active COFs, albeit with high capacity, are often confined to their sloping and low redox potential (&lt;0.8\u00a0V) caused by high molecular orbital energy levels (HOMO\/LUMO) of active moieties. Here we report a capacity\u2010voltage trade\u2010off\u2010breaking design of COFs by pairing low\u2010HOMO trithiophene donor (\u22126.04\u00a0eV) with low\u2010LUMO trinitrile acceptor (\u22123.82\u00a0eV) via robust olefin linkages (TN\u2010COF), using high\u2010LUMO triazine acceptor (\u22121.75\u00a0eV) as the counterpart (TA\u2010COF). The tri(thiophene\u2010nitrile) donor\u2010acceptor enables low HOMO\/LUMO energy levels (\u22123.98\/\u22125.94\u00a0eV) for TN\u2010COF cathode, thus unlocking a flat and high redox potential of 1.2\u00a0V compared to TA\u2010COF (0.9\u00a0V). An 18\u2010electron CF\n                    <jats:sub>3<\/jats:sub>\n                    SO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    \/NH\n                    <jats:sub>4<\/jats:sub>\n                    <jats:sup>+<\/jats:sup>\n                    (de)coordination process is activated per hexagonal tri(thiophene\u2010nitrile) unit in TN\u2010COF cathode with ultralow activation energy (0.17\u00a0eV). This facilitates 98.2% utilization of C\u2212S\/C\u2261N active sites to liberate high capacity of 335 mAh g\n                    <jats:sup>\u22121<\/jats:sup>\n                    (vs. 80.1%\/268 mAh g\n                    <jats:sup>\u22121<\/jats:sup>\n                    for TA\u2010COF). The ideal combination of high voltage and capacity gives TN\u2010COF cathode superior energy density (402\u00a0Wh kg\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) and ultralong life (70,000 cycles). This finding widens the design philosophy of high\u2010voltage\u2010capacity COFs via HOMO\/LUMO energy engineering for advanced ZOBs.\n                  <\/jats:p>","DOI":"10.1002\/anie.202525690","type":"journal-article","created":{"date-parts":[[2026,2,6]],"date-time":"2026-02-06T07:48:42Z","timestamp":1770364122000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":15,"title":["Tri(Thiophene\u2010Nitrile) Covalent Organic Frameworks With Low HOMO\/LUMO Donor\/Acceptor for High\u2010Potential\u2010Plateau Zinc Batteries"],"prefix":"10.1002","volume":"65","author":[{"given":"Pingxuan","family":"Liu","sequence":"first","affiliation":[{"name":"Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering Tongji University  Shanghai P. R. 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