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To this end, this study proposes an anthraquinone engineering strategy that aims to simultaneously enhance both structural stability and catalytic efficiency of organic semiconductors for photocatalysis. Specifically, 1,3,5\u2010tri(thiophen\u20102\u2010yl)benzene (TTB)\u2010based porous aromatic frameworks (PAFs) (TTB\u2010PAFs) are optimized by linking anthraquinone fragments via carbon\u2010carbon bond formation. The unique electron distribution, abundant active sites, nanotube\u2010like micromorphology, and robust carbon\u2010carbon bonding character of the optimized TTB\u2010PAF jointly facilitate the charge separation\/transfer, mass transportation, and stability during photocatalysis. Remarkably, these result in the optimal C\u2500H cyanation of tertiary amines over the PAF\u2010396 photocatalyst, achieving excellent yields (up to 99%), good substrate adaptability (18 examples), and good recyclability (10 cycles), thereby surpassing the performance of reported porous organic semiconductor materials under similar conditions. Furthermore, PAF\u2010396 also achieves efficient photosynthesis of hydrogen peroxide (H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    ) with a high synthesis rate of 5154 \u00b5mol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    from air and water without a sacrificial reagent under blue LED lamp irradiation.\n                  <\/jats:p>","DOI":"10.1002\/anie.6087657","type":"journal-article","created":{"date-parts":[[2026,7,6]],"date-time":"2026-07-06T08:21:47Z","timestamp":1783326107000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Anthraquinone\u2010Engineered Thiophene\u2010Based Nanotube\u2010Like Porous Aromatic Framework as a Robust and Efficient Bifunctional Photocatalyst for C\u2500H Cyanation of Tertiary Amines and Hydrogen Peroxide Generation"],"prefix":"10.1002","volume":"65","author":[{"given":"Bingxin","family":"Jia","sequence":"first","affiliation":[{"name":"Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education and Faculty of Chemistry Northeast Normal University  Changchun People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"He","family":"Wang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education and Faculty of Chemistry Northeast Normal University  Changchun People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4235-4662","authenticated-orcid":false,"given":"Xin","family":"Tao","sequence":"additional","affiliation":[{"name":"Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education and Faculty of Chemistry Northeast Normal 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