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Herein, two rationally designed thiophene\u2010rich monomers enable the effective coupling of thiophene and benzothiadiazole units within the same COF materials, yielding D\u2013A type COFs with\n                    <jats:bold>bex<\/jats:bold>\n                    topological structures (TTB\u2010COF and TTP\u2010COF). By modulating the central unit, the intramolecular built\u2010in electric field is enhanced, and the rotational freedom of thiophene units is also constrained, leading to a wavy structure in the monolayer COF, which significantly improves the material's photocatalytic performance. Using 2,2\u2032\u2010bipyridine as an additive, TTB\u2010COF\u2010Co achieves a high CO production rate of 28.0 mmol\u00a0g\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00a0h\n                    <jats:sup>\u22121<\/jats:sup>\n                    with a selectivity of 88.4% in the presence of the photosensitizer [Ru(bpy)\n                    <jats:sub>3<\/jats:sub>\n                    ]Cl\n                    <jats:sub>2<\/jats:sub>\n                    \u00b76H\n                    <jats:sub>2<\/jats:sub>\n                    O and the sacrificial agent triethanolamine (TEOA), being one of the best performances among COF\u2010based catalysts. Analysis of the cumulative free energy change diagrams reveals that TTB\u2010COF\u2010Co lowers the energy barrier of the rate\u2010determining step in CO\n                    <jats:sub>2<\/jats:sub>\n                    photoreduction, thereby demonstrating superior photocatalytic performance. This work provides a referable design strategy for constructing high\u2010performance COF\u2010based photocatalysts for CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction.\n                  <\/jats:p>","DOI":"10.1002\/anie.5240027","type":"journal-article","created":{"date-parts":[[2026,6,9]],"date-time":"2026-06-09T11:49:23Z","timestamp":1781005763000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Synergistic Electronic and Steric Engineering of Thiophene Donors in Covalent Organic Frameworks for Efficient CO\n                    <sub>2<\/sub>\n                    Photoconversion"],"prefix":"10.1002","volume":"65","author":[{"given":"Hanwen","family":"Wang","sequence":"first","affiliation":[{"name":"Department of Polymer Science and Engineering State Key Laboratory of Silicon and Advanced Semiconductor Materials Zhejiang University  Hangzhou 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