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As these materials are formed via endothermic or exothermic equilibria, their thermal response is challenging to control without drastically changing the nature of the chemistry used to join them. In this study, we introduce a novel class of PSHs utilizing the intercalation of double\u2010stranded DNA (dsDNA) as the primary dynamic non\u2010covalent interaction. The resulting dsDNA intercalating supramolecular hydrogels (DISHs) can be tuned to exhibit both endothermically or exothermically driven binding through strategic selection of intercalators. Bifunctional polyethylene glycol (M\n                    <jats:sub>W<\/jats:sub>\n                    ~2000\u2005Da) capped with intercalators of varying hydrophobicity, charge, and size (acridine, psoralen, thiazole orange, and phenanthridine) produced DISHs with comparable moduli (500\u20131000\u2005Pa), but unique thermal viscoelastic responses. Notably, acridine\u2010based cross\u2010linkers displayed invariant and even increasing relaxation times with temperature, suggesting an endothermic binding mechanism. This methodology expands the set of structure\u2010properties available to biomass\u2010derived DNA biomaterials and promises a new material system where a broad set of thermal and viscoelastic responses can be obtained due to the sheer number and variety of intercalating molecules.\n                  <\/jats:p>","DOI":"10.1002\/anie.202411115","type":"journal-article","created":{"date-parts":[[2024,8,5]],"date-time":"2024-08-05T14:53:28Z","timestamp":1722869608000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":11,"title":["DNA\u2010Intercalating Supramolecular Hydrogels for Tunable Thermal and Viscoelastic Properties"],"prefix":"10.1002","volume":"63","author":[{"given":"Shaina M.","family":"Hughes","sequence":"first","affiliation":[{"name":"Department of Chemistry, College of Engineering and Physical Science University of New Hampshire  23 Academic Way, Parsons Hall Durham NH 03824 United States of America"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Aylin","family":"Aykanat","sequence":"additional","affiliation":[{"name":"Department of Chemistry, College of Engineering and Physical Science University of New Hampshire  23 Academic Way, Parsons Hall Durham NH 03824 United States of America"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Nicholas G.","family":"Pierini","sequence":"additional","affiliation":[{"name":"Department of Chemistry, College of Engineering and Physical Science University of New Hampshire  23 Academic Way, Parsons Hall Durham NH 03824 United States of America"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wynter A.","family":"Paiva","sequence":"additional","affiliation":[{"name":"Department of Chemistry, College of Engineering and Physical Science University of New Hampshire  23 Academic Way, Parsons Hall Durham NH 03824 United States of America"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"April A.","family":"Weeks","sequence":"additional","affiliation":[{"name":"Department of Chemistry, College of Engineering and Physical Science University of New Hampshire  23 Academic Way, Parsons Hall Durham NH 03824 United States of America"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Austin S.","family":"Edwards","sequence":"additional","affiliation":[{"name":"Department of Chemistry, College of Engineering and Physical Science University of New Hampshire  23 Academic Way, Parsons Hall Durham NH 03824 United States of America"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Owen C.","family":"Durant","sequence":"additional","affiliation":[{"name":"Department of Chemistry, College of Engineering and Physical Science University of New Hampshire  23 Academic Way, Parsons Hall Durham NH 03824 United States of America"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4256-0826","authenticated-orcid":false,"given":"Nathan J.","family":"Oldenhuis","sequence":"additional","affiliation":[{"name":"Department of Chemistry, College of Engineering and Physical Science University of New Hampshire  23 Academic Way, Parsons Hall Durham NH 03824 United States of America"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2024,9,29]]},"reference":[{"key":"e_1_2_3_1_1","doi-asserted-by":"publisher","DOI":"10.1039\/c2cs35264h"},{"key":"e_1_2_3_2_1","doi-asserted-by":"publisher","DOI":"10.1007\/978-981-10-6881-2_2"},{"key":"e_1_2_3_3_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201806912"},{"key":"e_1_2_3_4_1","first-page":"1","volume":"2022","author":"Webber M. 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