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Herein, TpAQ\u2010TZ COF and TpAR\u2010TZ COF, featuring thiazole linkages, were synthesized by combining 1,3,5\u2010tricarboxylcarboxaldehyde (Tp), sulfur (S\n                    <jats:sub>8<\/jats:sub>\n                    ), and direct hydrogen atom transfer (\n                    <jats:italic>d<\/jats:italic>\n                    \u2010HAT) components (2,6\u2010diaminoanthraquinone, AQ; 2,6\u2010diaminoanthrone, AR). The TpAQ\u2010TZ COF demonstrates impressive photocatalytic activity, achieving a 93% yield for phthalan oxidation under heterogeneous conditions\u2014a rare example of photocatalytic C(sp\n                    <jats:sup>3<\/jats:sup>\n                    )\u2500H bond oxidation in water under ambient conditions. Theoretical calculations reveal enhanced hydrogen atom abstraction capability coming from the increased number of\n                    <jats:italic>d<\/jats:italic>\n                    \u2010HAT catalytic sites. Moreover, BdAQ\u2010TZ COF and HbAQ\u2010TZ COF were prepared by replacing Tp with 2,4\u2010dihydroxy\u20101,3,5\u2010triformylbenzene (Bd) or 2\u2010hydroxy\u20101,3,5\u2010triformylbenzene (Hb), respectively. Dipole moment calculations and femtosecond transient absorption spectroscopy show that the increased number of hydroxyl groups on the benzene\u20101,3,5\u2010tricarbaldehyde monomer improves the charge separation efficiency within the three COFs, thereby accounting for the enhanced photocatalytic activity of TpAQ\u2010TZ COF. This work opens up new opportunities for designing highly active photocatalysts by using the synergistic effects of\n                    <jats:italic>d<\/jats:italic>\n                    \u2010HAT, O\n                    <jats:sub>2<\/jats:sub>\n                    <jats:sup>\u2022\u2212<\/jats:sup>\n                    , and\n                    <jats:sup>1<\/jats:sup>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    within anthraquinone\u2010based donor\u2013acceptor COF platforms, offering a sustainable route for the oxidation of C(sp\n                    <jats:sup>3<\/jats:sup>\n                    )\u2500H bonds under environmentally friendly conditions.\n                  <\/jats:p>","DOI":"10.1002\/anie.202517694","type":"journal-article","created":{"date-parts":[[2025,10,3]],"date-time":"2025-10-03T11:16:02Z","timestamp":1759490162000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Anthraquinone\u2010Based Donor\u2013Acceptor Covalent Organic Frameworks with Thiazole Linkages to Enhance Direct Hydrogen Atom Transfer and Charge Separation in Photocatalytic Oxidation of C(sp\n                    <sup>3<\/sup>\n                    )\u2500H Bonds"],"prefix":"10.1002","volume":"64","author":[{"given":"Jie","family":"Guo","sequence":"first","affiliation":[{"name":"Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction Ministry of Education College of Chemistry Central China Normal University  Wuhan 430079 P.R. China"}]},{"given":"Xu\u2010Hang","family":"Zhong","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications College of Chemistry and Materials Science Jinan University  Guangzhou 510632 P.R. China"}]},{"given":"Li","family":"Rao","sequence":"additional","affiliation":[{"name":"Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction Ministry of Education College of Chemistry Central China Normal University  Wuhan 430079 P.R. China"}]},{"given":"Bing\u2010Zhe","family":"Wang","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications College of Chemistry and Materials Science Jinan University  Guangzhou 510632 P.R. China"}]},{"given":"Zhuo","family":"Chen","sequence":"additional","affiliation":[{"name":"Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction Ministry of Education College of Chemistry Central China Normal University  Wuhan 430079 P.R. China"}]},{"given":"Yu","family":"Zhang","sequence":"additional","affiliation":[{"name":"Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction Ministry of Education College of Chemistry Central China Normal University  Wuhan 430079 P.R. China"}]},{"given":"Tao","family":"Wu","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications College of Chemistry and Materials Science Jinan University  Guangzhou 510632 P.R. China"}]},{"given":"S\u00f3nia A. C.","family":"Carabineiro","sequence":"additional","affiliation":[{"name":"LAQV\u2010REQUIMTE Department of Chemistry NOVA School of Science and Technology Universidade NOVA de Lisboa  Caparica 2829\u2010516 Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8639-2978","authenticated-orcid":false,"given":"Li\u2010Li","family":"Wen","sequence":"additional","affiliation":[{"name":"Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction Ministry of Education College of Chemistry Central China Normal University  Wuhan 430079 P.R. China"}]},{"given":"Chun\u2010Ying","family":"Duan","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Coordination Chemistry Nanjing University  Nanjing 210093 P.R. China"}]}],"member":"311","published-online":{"date-parts":[[2025,10,3]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.0c09157"},{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c12724"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.chempr.2025.102442"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929-017-0001-5"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c00950"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202408428"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.4c03099"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41893-021-00682-x"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c14254"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.0c05507"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.1c00263"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201800818"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.accounts.5c00370"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929-019-0357-9"},{"key":"e_1_2_8_15_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.2c09366"},{"key":"e_1_2_8_16_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.2c06432"},{"key":"e_1_2_8_17_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c02703"},{"key":"e_1_2_8_18_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-024-44833-y"},{"key":"e_1_2_8_19_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41563-025-02281-z"},{"key":"e_1_2_8_20_1","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.201802088"},{"key":"e_1_2_8_21_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.1120411"},{"key":"e_1_2_8_22_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2022.214889"},{"key":"e_1_2_8_23_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c06113"},{"key":"e_1_2_8_24_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41557-024-01595-w"},{"key":"e_1_2_8_25_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.adr0936"},{"key":"e_1_2_8_26_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202303129"},{"key":"e_1_2_8_27_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202307991"},{"key":"e_1_2_8_28_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202502943"},{"key":"e_1_2_8_29_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202416240"},{"key":"e_1_2_8_30_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsami.5c01437"},{"key":"e_1_2_8_31_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202425017"},{"key":"e_1_2_8_32_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-024-51878-6"},{"key":"e_1_2_8_33_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.2c01030"},{"key":"e_1_2_8_34_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.inorgchem.2c00441"},{"key":"e_1_2_8_35_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.2c09348"},{"key":"e_1_2_8_36_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.3c02220"},{"key":"e_1_2_8_37_1","doi-asserted-by":"publisher","DOI":"10.1039\/D3OB02122J"},{"key":"e_1_2_8_38_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.0c03418"},{"key":"e_1_2_8_39_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c13172"},{"key":"e_1_2_8_40_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja409421d"},{"key":"e_1_2_8_41_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.8b05830"},{"key":"e_1_2_8_42_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202302276"},{"key":"e_1_2_8_43_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202422940"},{"key":"e_1_2_8_44_1","doi-asserted-by":"publisher","DOI":"10.1002\/cctc.202300893"},{"key":"e_1_2_8_45_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.jcim.3c00776"},{"key":"e_1_2_8_46_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.jmedchem.1c02007"},{"key":"e_1_2_8_47_1","doi-asserted-by":"publisher","DOI":"10.1038\/s44160-022-00125-1"},{"key":"e_1_2_8_48_1","doi-asserted-by":"publisher","DOI":"10.1201\/9781420007282"},{"key":"e_1_2_8_49_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.abd8408"},{"key":"e_1_2_8_50_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c01273"},{"key":"e_1_2_8_51_1","volume":"64","author":"Tang Y.\u2010Y.","year":"2024","journal-title":"Angew. 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