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Nevertheless, their efficiency is often constrained by the presence of deep trap states that lead to rapid charge carrier recombination. Here, we fine\u2010tune the p\u2013\u03c0 resonance of pyrene\u2010based COFs by functionalizing the 5,6 positions of benzo[\n                    <jats:italic>c<\/jats:italic>\n                    ][1,2,5]thiadiazole\u20104,7\u2010diyl)dibenzaldehyde (BT) with electron\u2010withdrawing (\u2013F), mixed (\u2013F\/\u2013OCH\n                    <jats:sub>3<\/jats:sub>\n                    ), and electron\u2010donating (\u2013OCH\n                    <jats:sub>3<\/jats:sub>\n                    ) groups followed by condensation with 4,4\u2032,4\u2033,4\u2034\u2010(pyrene\u20101,3,6,8\u2010tetrayl)tetraaniline to afford BTCOF\u20102F, BTCOF\u2010Mix, and BTCOF\u20102OCH\n                    <jats:sub>3<\/jats:sub>\n                    , respectively. The mixed p\u2013\u03c0 resonance strengthens the internal electric field, reduces the exciton binding energy to 62.06 meV, and generates long\u2010lived shallow trap states with a lifetime up to 1574.6\u00a0ps for BTCOF\u2010Mix. As a result, BTCOF\u2010Mix photocatalysis realizes a U(VI) uptake of 1600.1\u00a0mg g\n                    <jats:sup>\u22121<\/jats:sup>\n                    and a rate constant of 0.084 min\n                    <jats:sup>\u22121<\/jats:sup>\n                    , outperforming those of BTCOF\u20102F (1090.2\u00a0mg g\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) and BTCOF\u20102OCH\n                    <jats:sub>3<\/jats:sub>\n                    (1245.2\u00a0mg g\n                    <jats:sup>\u22121<\/jats:sup>\n                    ). Notably, BTCOF\u2010Mix achieves over 90% selectivity in the presence of competing ions and more than 99% reduction of U(VI) and ensuing recovery by visible\u2010light photocatalysis from real mining wastewater. This work demonstrates that balancing p\u2013\u03c0 resonance constitutes a viable approach for modulation of the trap state energetics of COF photocatalysis toward solar\u2010driven reduction and recovery of radioactive ions in aquatic environments.\n                  <\/jats:p>","DOI":"10.1002\/smll.75531","type":"journal-article","created":{"date-parts":[[2026,9,11]],"date-time":"2026-09-11T06:53:01Z","timestamp":1789109581000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Mixed p\u2013\u03c0 Resonance in Pyrene\u2010Based Covalent Organic Frameworks: Shallow Trap Charge Dynamics for Efficient Photocatalysis in Reduction of U(VI)"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-3902-3093","authenticated-orcid":false,"given":"Weijie","family":"Zhang","sequence":"first","affiliation":[{"name":"Hunan Provincial Key Laboratory of Environmental Catalysis &amp; Waste Recycling College of Materials and Chemical Engineering Hunan Institute of Engineering  Xiangtan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinxu","family":"Deng","sequence":"additional","affiliation":[{"name":"Hunan Provincial Key Laboratory of Environmental Catalysis &amp; Waste Recycling College of Materials and Chemical Engineering Hunan Institute of Engineering  Xiangtan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuxi","family":"Liu","sequence":"additional","affiliation":[{"name":"Hunan Provincial Key Laboratory of Environmental Catalysis &amp; Waste Recycling College of Materials and Chemical Engineering Hunan Institute of Engineering  Xiangtan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yang","family":"Ma","sequence":"additional","affiliation":[{"name":"Hunan Provincial Key Laboratory of Environmental Catalysis &amp; Waste Recycling College of Materials and Chemical Engineering Hunan Institute of Engineering  Xiangtan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0000-9371-6558","authenticated-orcid":false,"given":"Kanghui","family":"Xiong","sequence":"additional","affiliation":[{"name":"Hubei Key Lab on Organic and Polymeric Optoelectronic Materials College of Chemistry and Molecular Sciences Wuhan University  Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4192-2306","authenticated-orcid":false,"given":"Hai","family":"Yang","sequence":"additional","affiliation":[{"name":"Hunan Provincial Key Laboratory of Environmental Catalysis &amp; Waste Recycling College of Materials and Chemical Engineering Hunan Institute of Engineering  Xiangtan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7479-9044","authenticated-orcid":false,"given":"Xianjun","family":"Lang","sequence":"additional","affiliation":[{"name":"Hubei Key Lab on Organic and 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