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Herein, we present a comprehensive strategy for the synthesis of extended \u03c0\u2010conjugated COFs via a one\u2010pot tandem Scholl cyclization\u2010dehydrogenation reaction. The extended \u03c0\u2010conjugated COFs are constructed by planar covalent bonds, in which imine linkers are converted to imine\u2010cyclized counterparts, resulting in all chemical bonds conjugatively connected throughout the framework. Subsequently, benzene units are substituted with naphthalene units to yield an even more highly extended \u03c0\u2010conjugated framework. These approaches ensure that delocalized electrons efficiently transport across the COF framework with extended \u03c0\u2010conjugation, resulting in extended\u2010range light absorption, improved electron\u2010hole separation, and more efficient charge\u2010carrier utilization under visible\u2010light irradiation. Notably, the extended \u03c0\u2010conjugated COFs exhibit remarkable photocatalytic performance in uranium(VI) removal from contaminated water sources, surpassing the performance of electron\u2010deficient p\u2010\u03c0\u2010conjugated counterparts. These findings demonstrate a new general design strategy for the synthesis of highly\u2010conjugated COF photocatalysts. The strategy is expected to provide new insights into the rational design of high\u2010performance COFs for applications in photocatalysis, including water\u2010source decontamination and potentially numerous other applications.<\/jats:p>","DOI":"10.1002\/smll.74554","type":"journal-article","created":{"date-parts":[[2026,7,11]],"date-time":"2026-07-11T15:40:48Z","timestamp":1783784448000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Rational Synthesis of Extended \u03c0\u2010Conjugated Covalent Organic Frameworks for Enhanced Photocatalytic Uranium(VI) Removal"],"prefix":"10.1002","volume":"22","author":[{"given":"Juyao","family":"Zhang","sequence":"first","affiliation":[{"name":"College of Environmental Science and Engineering North China Electric Power University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mengjie","family":"Hao","sequence":"additional","affiliation":[{"name":"College of Environmental Science and Engineering North China Electric Power University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyue","family":"Zhang","sequence":"additional","affiliation":[{"name":"College of Environmental Science and Engineering North China Electric Power University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Muliang","family":"Xiao","sequence":"additional","affiliation":[{"name":"College of Environmental Science and Engineering North China Electric Power University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yinghui","family":"Xie","sequence":"additional","affiliation":[{"name":"College of Environmental Science and Engineering North China Electric Power University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ruining","family":"Cao","sequence":"additional","affiliation":[{"name":"College of Environmental Science and Engineering North China Electric Power University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"He","family":"Gu","sequence":"additional","affiliation":[{"name":"College of Environmental Science and Engineering North China Electric Power University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaolu","family":"Liu","sequence":"additional","affiliation":[{"name":"College of Environmental Science and Engineering North China Electric Power University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6745-642X","authenticated-orcid":false,"given":"Hui","family":"Yang","sequence":"additional","affiliation":[{"name":"College of Environmental Science and Engineering North China Electric Power University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Geoffrey I. 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