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However, conventional structural modifications fail to systematically tune oxygen adsorption geometry and interfacial electronic coupling. Here, we report a linkage\u2010angle engineering strategy that alters the bonding positions of reactive aldehyde groups to fabricate three regioisomeric COFs with predefined backbone dihedral angles of 180\u00b0, 120\u00b0, and 60\u00b0. The angle\u2011driven regioisomeric effect induces considerable differences in dipole moments together with uneven charge distribution. These collective structural features remodel oxygen\u2011surface interactions and modulate the intrinsic catalytic kinetics. Theoretical calculations confirm that the compact 60\u00b0 framework of\n                    <jats:bold>\n                      <jats:italic>o<\/jats:italic>\n                      \u2010TPDA\u2010COF\n                    <\/jats:bold>\n                    reconstructs confined pore interfacial microenvironments. Unlike the Griffiths\u2011type oxygen adsorption favored in its angular analogues, molecular oxygen preferentially adopts the Pauling configuration within\n                    <jats:bold>\n                      <jats:italic>o<\/jats:italic>\n                      \u2010TPDA\u2010COF\n                    <\/jats:bold>\n                    to stabilize OOH* intermediates. Consequently, the optimal\n                    <jats:bold>\n                      <jats:italic>o<\/jats:italic>\n                      \u2010TPDA\u2010COF\n                    <\/jats:bold>\n                    reaches an excellent H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    productivity of 12.82\u00a0mol g\n                    <jats:sub>cat<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    and a Faradaic efficiency (FE) of 91.64%. This work realizes controllable modulation of oxygen\u2011adsorption behaviors in COF\u2011based 2e\n                    <jats:sup>\u2013<\/jats:sup>\n                    oxygen reduction, delivering a novel geometry\u2011oriented design paradigm for porous electrocatalytic frameworks.\n                  <\/jats:p>","DOI":"10.1002\/anie.5704652","type":"journal-article","created":{"date-parts":[[2026,10,13]],"date-time":"2026-10-13T06:12:44Z","timestamp":1791871964000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Tailoring Backbone Angles of Regioisomeric Covalent Organic Frameworks: Distinct O\n                    <sub>2<\/sub>\n                    Adsorption Modes Enabling Efficient H\n                    <sub>2<\/sub>\n                    O\n                    <sub>2<\/sub>\n                    Electrosynthesis"],"prefix":"10.1002","author":[{"given":"Yali","family":"Xing","sequence":"first","affiliation":[{"name":"State Key Laboratory of Bio\u2010fibers and Eco\u2010textiles Institute of Marine Biobased Materials College of Materials Science and Engineering Qingdao University  Qingdao P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuo","family":"Chen","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Bio\u2010fibers and Eco\u2010textiles Institute of Marine Biobased Materials College of Materials Science and Engineering Qingdao University  Qingdao P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Han","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Bio\u2010fibers and Eco\u2010textiles Institute of Marine Biobased Materials College of Materials Science and Engineering Qingdao University  Qingdao P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xue","family":"Zhang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Bio\u2010fibers and Eco\u2010textiles Institute of Marine Biobased Materials College of Materials Science and Engineering Qingdao University  Qingdao P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ning","family":"Sun","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Bio\u2010fibers and Eco\u2010textiles Institute of Marine Biobased Materials College of Materials Science and Engineering Qingdao University  Qingdao P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chengjing","family":"Fu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Bio\u2010fibers and Eco\u2010textiles Institute of Marine Biobased Materials College of Materials Science and Engineering Qingdao University  Qingdao P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9899-1820","authenticated-orcid":false,"given":"Xiaojing","family":"Long","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Bio\u2010fibers and Eco\u2010textiles Institute of Marine Biobased Materials College of Materials Science and Engineering Qingdao University  Qingdao P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,10,12]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.4c00950"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202412386"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2024.216240"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202501494"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2025.217558"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202420236"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2025.216972"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1038\/s44160\u2010024\u201000722\u20102"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010026\u201071584\u20109"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010025\u201064901\u20101"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202510604"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.31635\/renewables.025.202500084"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.6c00875"},{"key":"e_1_2_8_15_1","doi-asserted-by":"publisher","DOI":"10.1039\/D4CS00521J"},{"key":"e_1_2_8_16_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202414490"},{"key":"e_1_2_8_17_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202416401"},{"key":"e_1_2_8_18_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41565\u2010024\u201001815\u2010x"},{"key":"e_1_2_8_19_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010025\u201060467\u20100"},{"key":"e_1_2_8_20_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010025\u201065887\u20106"},{"key":"e_1_2_8_21_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.1168049"},{"key":"e_1_2_8_22_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929\u2010018\u20100044\u20102"},{"key":"e_1_2_8_23_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.1120411"},{"key":"e_1_2_8_24_1","doi-asserted-by":"publisher","DOI":"10.1039\/D0CS00017E"},{"key":"e_1_2_8_25_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c01131"},{"key":"e_1_2_8_26_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202307459"},{"key":"e_1_2_8_27_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202513499"},{"key":"e_1_2_8_28_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010026\u201070591\u20100"},{"key":"e_1_2_8_29_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.73311"},{"key":"e_1_2_8_30_1","doi-asserted-by":"publisher","DOI":"10.1002\/ece2.32"},{"key":"e_1_2_8_31_1","doi-asserted-by":"publisher","DOI":"10.1039\/D5CS01537E"},{"key":"e_1_2_8_32_1","doi-asserted-by":"publisher","DOI":"10.1002\/ange.202203250"},{"key":"e_1_2_8_33_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202523668"},{"key":"e_1_2_8_34_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.accounts.5c00086"},{"key":"e_1_2_8_35_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41563\u2010025\u201002281\u2010z"},{"key":"e_1_2_8_36_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202511092"},{"key":"e_1_2_8_37_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202305355"},{"key":"e_1_2_8_38_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010025\u201063997\u20109"},{"key":"e_1_2_8_39_1","doi-asserted-by":"publisher","DOI":"10.1038\/s44160\u2010026\u201001123\u20103"},{"key":"e_1_2_8_40_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.adu2527"},{"key":"e_1_2_8_41_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.5815461"},{"key":"e_1_2_8_42_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010026\u201070165\u20100"},{"key":"e_1_2_8_43_1","doi-asserted-by":"publisher","DOI":"10.1039\/D5EE01407G"},{"key":"e_1_2_8_44_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202524265"},{"key":"e_1_2_8_45_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202500913"},{"key":"e_1_2_8_46_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202516067"},{"key":"e_1_2_8_47_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010026\u201070311\u20108"},{"key":"e_1_2_8_48_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202500644"},{"key":"e_1_2_8_49_1","doi-asserted-by":"publisher","DOI":"10.1016\/S1872\u20102067(23)64457\u20102"},{"key":"e_1_2_8_50_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202500063"},{"key":"e_1_2_8_51_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.6c02577"},{"key":"e_1_2_8_52_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacsau.3c00088"},{"key":"e_1_2_8_53_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010022\u201029814\u20103"},{"key":"e_1_2_8_54_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202500945"},{"key":"e_1_2_8_55_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.esci.2026.1005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