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However, their synthesis is hampered by the scarcity of redox-active monomers and the difficulty of functionalizing as-synthesized frameworks without compromising crystallinity. Here, we introduce a reductive N-methylation strategy that enables the universal and mild conversion of imine-linked COFs into crystalline tertiary amine-linked frameworks (NMe-COFs). The method preserves structural order while imparting strong electron-donating and redox-responsive properties. Among the NMe-COFs, COF-300-NMe exhibits an 11-fold increase in iodine uptake with a distinct gate-opening adsorption profile\u2500a behavior that computational studies attribute to enhanced framework flexibility and raised electronic energy levels. Furthermore, incorporation of the electron acceptor 7,7,8,8-tetracyanoquinodimethane into COF-300-NMe yields a charge-transfer complex exhibiting distinct spin signatures. This work establishes a versatile postsynthetic linkage conversion strategy, paving the way toward stimuli-responsive soft COFs and purely organic spin-active materials.<\/jats:p>","DOI":"10.1021\/jacs.6c01356","type":"journal-article","created":{"date-parts":[[2026,7,16]],"date-time":"2026-07-16T13:38:28Z","timestamp":1784209108000},"page":"30793-30801","source":"Crossref","is-referenced-by-count":0,"title":["Facile Fabrication\nof Redox-Active Covalent Organic\nFrameworks via Reductive\n                    <i>N<\/i>\n                    -methylation"],"prefix":"10.1021","volume":"148","author":[{"given":"Jinquan","family":"Suo","sequence":"first","affiliation":[{"name":"Jilin University , , ,","place":["Changchun, P. R. China, 130012"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fengqian","family":"Chen","sequence":"additional","affiliation":[{"name":"Jilin University , , ,","place":["Changchun, P. R. China, 130012"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bin","family":"Zhao","sequence":"additional","affiliation":[{"name":"Jilin University , , ,","place":["Changchun, P. R. China, 130012"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hui","family":"Li","sequence":"additional","affiliation":[{"name":"Jilin University , , ,","place":["Changchun, P. R. China, 130012"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2341-6397","authenticated-orcid":true,"given":"Valentin","family":"Valtchev","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , 189 Songling Road , ,","place":["Qingdao, P. R. China, 266101"]},{"name":"Normandie Universite\u0301, CNRS , , 6 Marechal Juin , ,","place":["Caen, France, 14050"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shilun","family":"Qiu","sequence":"additional","affiliation":[{"name":"Jilin University , , ,","place":["Changchun, P. R. China, 130012"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3365-5508","authenticated-orcid":true,"given":"Qianrong","family":"Fang","sequence":"additional","affiliation":[{"name":"Jilin University , , ,","place":["Changchun, P. R. 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Am. Chem. Soc."},{"issue":"23","key":"2026073021324916100_cit4","doi-asserted-by":"publisher","first-page":"6814","DOI":"10.1002\/anie.201501706","article-title":"Radical Covalent Organic Frameworks:\nA General Strategy to Immobilize Open-Accessible Polyradicals for\nHigh-Performance Capacitive Energy Storage","volume":"54","author":"Xu","year":"2015","journal-title":"Angew. Chem., Int. Ed."},{"issue":"1","key":"2026073021324916100_cit5","doi-asserted-by":"publisher","first-page":"16","DOI":"10.1021\/jacs.9b08147","article-title":"Phenazine-Based\nCovalent Organic Framework Cathode\nMaterials with High Energy and Power Densities","volume":"142","author":"Vitaku","year":"2020","journal-title":"J. Am. Chem. Soc."},{"issue":"21","key":"2026073021324916100_cit6","doi-asserted-by":"publisher","first-page":"9434","DOI":"10.1021\/jacs.2c02196","article-title":"A Pyrene-4,5,9,10-Tetraone-Based\nCovalent Organic Framework Delivers High Specific Capacity as a Li-Ion\nPositive Electrode","volume":"144","author":"Gao","year":"2022","journal-title":"J. Am. Chem. Soc."},{"issue":"10","key":"2026073021324916100_cit7","doi-asserted-by":"publisher","first-page":"4168","DOI":"10.1002\/anie.201916360","article-title":"Redox-Active Two-Dimensional\nCovalent Organic Frameworks (COFs) for Selective Reductive Separation\nof Valence-Variable, Redox-Sensitive and Long-Lived Radionuclides","volume":"59","author":"Li","year":"2020","journal-title":"Angew. Chem., Int. 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Res."},{"issue":"12","key":"2026073021324916100_cit17","doi-asserted-by":"publisher","first-page":"881","DOI":"10.1038\/s41570-022-00437-y","article-title":"Imine and Imine-Derived\nLinkages\nin Two-Dimensional Covalent Organic Frameworks","volume":"6","author":"Qian","year":"2022","journal-title":"Nat. Rev. Chem."},{"issue":"48","key":"2026073021324916100_cit18","doi-asserted-by":"publisher","first-page":"15519","DOI":"10.1021\/jacs.6b08377","article-title":"Chemical\nConversion of Linkages in Covalent Organic\nFrameworks","volume":"138","author":"Waller","year":"2016","journal-title":"J. Am. Chem. Soc."},{"issue":"7","key":"2026073021324916100_cit19","doi-asserted-by":"publisher","first-page":"1696","DOI":"10.1016\/j.chempr.2018.05.003","article-title":"Covalent Organic\nFrameworks Linked by Amine Bonding for Concerted Electrochemical Reduction\nof CO2","volume":"4","author":"Liu","year":"2018","journal-title":"Chem"},{"issue":"1","key":"2026073021324916100_cit20","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-018-05462-4","article-title":"Facile Transformation of Imine Covalent\nOrganic Frameworks into Ultrastable\nCrystalline Porous Aromatic Frameworks","volume":"9","author":"Li","year":"2018","journal-title":"Nat.\nCommun."},{"issue":"41","key":"2026073021324916100_cit21","doi-asserted-by":"publisher","first-page":"9346","DOI":"10.1021\/jp054334s","article-title":"Aromatic Amines:\nA Comparison of Electron-Donor Strengths","volume":"109","author":"Kwon","year":"2005","journal-title":"J.\nPhys. Chem. 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Ed."},{"issue":"35","key":"2026073021324916100_cit28","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202208086","article-title":"Tuning the\nInterlayer Interactions of 2D Covalent Organic Frameworks Enables\nan Ultrastable Platform for Anhydrous Proton Transport","volume":"61","author":"Jiang","year":"2022","journal-title":"Angew. Chem., Int. Ed."},{"issue":"20","key":"2026073021324916100_cit29","doi-asserted-by":"publisher","first-page":"14145","DOI":"10.1021\/acs.inorgchem.9b02176","article-title":"Iodine Adsorption\nin a Redox-Active Metal\u2013Organic Framework: Electrical Conductivity\nInduced by Host\u2013Guest Charge-Transfer","volume":"58","author":"Zhang","year":"2019","journal-title":"Inorg. Chem."},{"issue":"8","key":"2026073021324916100_cit30","doi-asserted-by":"publisher","first-page":"3243","DOI":"10.1039\/D0CS01192D","article-title":"Adsorption of Iodine in Metal\u2013Organic\nFramework\nMaterials","volume":"51","author":"Zhang","year":"2022","journal-title":"Chem. Soc. Rev."},{"issue":"1","key":"2026073021324916100_cit31","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-020-19858-8","article-title":"Diverse Crystal\nSize Effects in Covalent Organic Frameworks","volume":"11","author":"Ma","year":"2020","journal-title":"Nat. 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