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Herein, the study has demonstrated that tuning the electronic properties of diketopyrrolopyrrole\u2010based donor\u2010acceptor covalent organic frameworks (COFs) enhances iodine trapping, improves charge transport, and strengthens iodine interactions \u2212 establishing a structure\u2010property relationship. This tuning is achieved by synthesizing COFs with the diketopyrrolopyrrole\u2010based linker 3,6\u2010bis(4\u2010(1,3\u2010dioxolan\u20102\u2010yl)phenyl)\u20102,5\u2010dihydropyrrolo[3,4\u2010c]pyrrole\u20101,4\u2010dione (DKP) in combination with either the electron acceptor 4,4\u2032,4\u2033\u2010(1,3,5\u2010triazine\u20102,4,6\u2010triyl)trianiline (TTT\u2010DKP) or the electron donor\n                    <jats:italic>\n                      N\n                      <jats:sub>1<\/jats:sub>\n                      ,N\n                      <jats:sub>1<\/jats:sub>\n                    <\/jats:italic>\n                    \u2010bis(4\u2010aminophenyl)benzene\u20101,4\u2010diamine (TAPA\u2010DKP) linkers. These COFs, with abundant sorption sites, thermal and chemical stability, and optimized pore environments, efficiently bind iodine in the vapor and solution phases. The TAPA\u2010DKP COF, containing electron\u2010donating moieties, showed a high iodine uptake of 3.52\u00a0g\/g, exceeding the 2.81\u00a0g\/g of the electron\u2010deficient TTT\u2010DKP in the vapor phase, both following pseudo\u2010second\u2010order kinetics. Density functional theory (DFT) calculations reveal adsorption sites showing that TAPA\u2010DKP COF binds I\n                    <jats:sub>2<\/jats:sub>\n                    more effectively via its electron\u2010rich moieties, highlighting the role of electronic property modulation in iodine adsorption.\n                  <\/jats:p>","DOI":"10.1002\/smll.202411199","type":"journal-article","created":{"date-parts":[[2025,3,11]],"date-time":"2025-03-11T17:49:39Z","timestamp":1741715379000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":26,"title":["Diketopyrrolopyrrole\u2010based Donor\u2013Acceptor Covalent Organic Frameworks for Iodine Capture"],"prefix":"10.1002","volume":"21","author":[{"given":"Bikash","family":"Mishra","sequence":"first","affiliation":[{"name":"Department of Chemical and Biological Sciences S. N. 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