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Such a situation can also occur in the preparation processes of supramolecular polymers formed in a solution. An effective strategy to address this issue is to prepare amorphous solid states by introducing a \u201ccoformer\u201d molecule capable of inhibiting the formation of an insoluble polymorph through co\u2010aggregation. Herein, inspired by the coformer approach, we demonstrated a solubility enhancement of a barbiturate \u03c0\u2010conjugated compound that can supramolecularly polymerize through six\u2010membered hydrogen\u2010bonded rosettes. Our newly synthesized supramolecular coformer molecule features a sterically demanding methyl group in the \u03c0\u2010conjugated unit of the parent molecule. Although the parent molecule exhibits low solubility in nonpolar solvents due to the formation of a crystalline polymorph comprising a tape\u2010like hydrogen\u2010bonded array prior to the supramolecular polymerization, mixing with the coformer compound enhanced the solubility by inhibiting mesoscopic organization of the tapes. The two monomers were then co\u2010polymerized into desired helicoidal supramolecular polymers through the formation of heteromeric rosettes.<\/jats:p>","DOI":"10.1002\/anie.202312516","type":"journal-article","created":{"date-parts":[[2023,9,22]],"date-time":"2023-09-22T05:06:12Z","timestamp":1695359172000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":22,"title":["A Coformer Approach for Supramolecular Polymerization at High Concentrations"],"prefix":"10.1002","volume":"62","author":[{"given":"Atsushi","family":"Isobe","sequence":"first","affiliation":[{"name":"Division of Advanced Science and Engineering Graduate School of Science and Engineering Chiba University  1-33 Yayoi-cho, Inage-ku 263-8522 Chiba Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Takashi","family":"Kajitani","sequence":"additional","affiliation":[{"name":"TC College Promotion Office Open Facility Center Tokyo Institute of Technology  4259 Nagatsuta, Midori-ku 226-8503 Yokohama Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4786-8603","authenticated-orcid":false,"given":"Shiki","family":"Yagai","sequence":"additional","affiliation":[{"name":"Institute for Advanced Academic Research (IAAR) Chiba University  1-33 Yayoi-cho, Inage-ku 263-8522 Chiba Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2023,10,9]]},"reference":[{"key":"e_1_2_7_1_1","unstructured":"\u00a0"},{"key":"e_1_2_7_2_2","doi-asserted-by":"publisher","DOI":"10.1093\/oso\/9780199655441.001.0001"},{"key":"e_1_2_7_3_2","doi-asserted-by":"crossref","first-page":"77","DOI":"10.1142\/9789814338769_0004","volume-title":"Crystal Engineering: A Textbook","author":"Desiraju G. 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