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Here we report the photocatalytic reduction of CO\u2082 to carbon monoxide, formate, and oxalate ions using a redox\u2010active phenazine\u2010based 2D covalent organic framework (<jats:bold>Phen\u2010COF<\/jats:bold>) and its phenazine monomer. Under similar irradiation conditions, <jats:bold>Phen\u2010COF<\/jats:bold> produced 2.9 times more CO, 11 times more formate, and 13 times more oxalate compared to equimolar amounts of the monomeric phenazine, demonstrating that the COF architecture enhances catalytic performance (TOF<jats:sub>COF<\/jats:sub>: 10<jats:sup>\u22127<\/jats:sup> s<jats:sup>\u22121<\/jats:sup> CO, 10<jats:sup>\u22128<\/jats:sup> s<jats:sup>\u22121<\/jats:sup> formate, and 10<jats:sup>\u221211<\/jats:sup> s<jats:sup>\u22121<\/jats:sup> oxalate). Structural analysis, including X\u2010ray diffraction and N\u2082 porosimetry, confirmed the COF's long\u2010range order and porosity. Mechanistic studies suggest a sequential formate\u2010to\u2010oxalate pathway, with CO and formate acting as intermediates. These results demonstrate the potential of the COF architecture to improve the performance of metal\u2010free, redox\u2010active aromatic systems such as phenazines to facilitate efficient and selective CO\u2082 conversion under mild conditions.<\/jats:p>","DOI":"10.1002\/anie.202502799","type":"journal-article","created":{"date-parts":[[2025,3,12]],"date-time":"2025-03-12T04:58:05Z","timestamp":1741755485000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":30,"title":["A Phenazine\u2010Based Two\u2010Dimensional Covalent Organic Framework for Photochemical CO<sub>2<\/sub> Reduction with Increased Selectivity for Two\u2010Carbon Products"],"prefix":"10.1002","volume":"64","author":[{"given":"Zoheb","family":"Hirani","sequence":"first","affiliation":[{"name":"Department of Chemistry Northwestern University  2145 Sheridan Road Evanston IL 60208 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Neil M.","family":"Schweitzer","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biological Engineering Northwestern University  2145 Sheridan Road Evanston IL 60208 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Edon","family":"Vitaku","sequence":"additional","affiliation":[{"name":"Department of Chemistry Northwestern University  2145 Sheridan Road Evanston IL 60208 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"William R.","family":"Dichtel","sequence":"additional","affiliation":[{"name":"Department of Chemistry Northwestern University  2145 Sheridan Road Evanston IL 60208 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,3,18]]},"reference":[{"key":"e_1_2_5_1_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.0c00478"},{"key":"e_1_2_5_2_1","doi-asserted-by":"publisher","DOI":"10.1002\/advs.201700194"},{"key":"e_1_2_5_3_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.jpcc.2c08963"},{"key":"e_1_2_5_4_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41563-020-0610-2"},{"key":"e_1_2_5_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.accounts.9b00496"},{"key":"e_1_2_5_6_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2021.214340"},{"key":"e_1_2_5_7_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jcou.2022.102056"},{"key":"e_1_2_5_8_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.8b00705"},{"key":"e_1_2_5_9_1","doi-asserted-by":"publisher","DOI":"10.1002\/cssc.201902061"},{"key":"e_1_2_5_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/er.6079"},{"key":"e_1_2_5_11_1","volume":"20","author":"Yuan Z.","year":"2024","journal-title":"Env. 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