Laura Rijns , Heleen Duijs , René P. M. Lafleur , Ruth Cardinaels , Anja R. A. Palmans , Patricia Y. W. Dankers , Lu Su
{"title":"具有可调机械和动态特性的分子工程超分子热致伸缩水凝胶。","authors":"Laura Rijns , Heleen Duijs , René P. M. Lafleur , Ruth Cardinaels , Anja R. A. Palmans , Patricia Y. W. Dankers , Lu Su","doi":"10.1021/acs.biomac.3c01357","DOIUrl":null,"url":null,"abstract":"<div><p>Synthetic supramolecular polymers and hydrogels in water are emerging as promising biomaterials due to their modularity and intrinsic dynamics. Here, we introduce temperature sensitivity into the nonfunctionalized benzene-1,3,5-tricarboxamide (<strong>BTA-EG</strong> <sub>\n4\n</sub>) supramolecular system by incorporating a poly(<em>N</em>-isopropylacrylamide)-functionalized (<strong>BTA-PNIPAM)</strong> moiety, enabling 3D cell encapsulation applications. The viscous and structural properties in the solution state as well as the mechanical and dynamic features in the gel state of <strong>BTA-PNIPAM/BTA-EG</strong> <sub>\n4\n</sub> mixtures were investigated and modulated. In the dilute state (<em>c</em> ∼μM), <strong>BTA-PNIPAM</strong> acted as a chain capper below the cloud point temperature (<em>T</em> <sub>cp</sub> = 24 °C) but served as a cross-linker above <em>T</em> <sub>cp</sub>. At higher concentrations (<em>c</em> ∼mM), weak or stiff hydrogels were obtained, depending on the <strong>BTA-PNIPAM/BTA-EG 4\n</strong> ratio. The mixture with the highest <strong>BTA-PNIPAM</strong> ratio was ∼100 times stiffer and ∼10 times less dynamic than <strong>BTA-EG</strong> <sub>\n4\n</sub> hydrogel. Facile cell encapsulation in 3D was realized by leveraging the temperature-sensitive sol–gel transition, opening opportunities for utilizing this hydrogel as an extracellular matrix mimic.</p></div><div><p><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (62KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></p></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"25 8","pages":"Pages 4686-4696"},"PeriodicalIF":5.4000,"publicationDate":"2024-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11323010/pdf/","citationCount":"0","resultStr":"{\"title\":\"Molecularly Engineered Supramolecular Thermoresponsive Hydrogels with Tunable Mechanical and Dynamic Properties\",\"authors\":\"Laura Rijns , Heleen Duijs , René P. M. Lafleur , Ruth Cardinaels , Anja R. A. Palmans , Patricia Y. W. Dankers , Lu Su\",\"doi\":\"10.1021/acs.biomac.3c01357\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Synthetic supramolecular polymers and hydrogels in water are emerging as promising biomaterials due to their modularity and intrinsic dynamics. Here, we introduce temperature sensitivity into the nonfunctionalized benzene-1,3,5-tricarboxamide (<strong>BTA-EG</strong> <sub>\\n4\\n</sub>) supramolecular system by incorporating a poly(<em>N</em>-isopropylacrylamide)-functionalized (<strong>BTA-PNIPAM)</strong> moiety, enabling 3D cell encapsulation applications. The viscous and structural properties in the solution state as well as the mechanical and dynamic features in the gel state of <strong>BTA-PNIPAM/BTA-EG</strong> <sub>\\n4\\n</sub> mixtures were investigated and modulated. In the dilute state (<em>c</em> ∼μM), <strong>BTA-PNIPAM</strong> acted as a chain capper below the cloud point temperature (<em>T</em> <sub>cp</sub> = 24 °C) but served as a cross-linker above <em>T</em> <sub>cp</sub>. At higher concentrations (<em>c</em> ∼mM), weak or stiff hydrogels were obtained, depending on the <strong>BTA-PNIPAM/BTA-EG 4\\n</strong> ratio. The mixture with the highest <strong>BTA-PNIPAM</strong> ratio was ∼100 times stiffer and ∼10 times less dynamic than <strong>BTA-EG</strong> <sub>\\n4\\n</sub> hydrogel. Facile cell encapsulation in 3D was realized by leveraging the temperature-sensitive sol–gel transition, opening opportunities for utilizing this hydrogel as an extracellular matrix mimic.</p></div><div><p><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (62KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></p></div>\",\"PeriodicalId\":30,\"journal\":{\"name\":\"Biomacromolecules\",\"volume\":\"25 8\",\"pages\":\"Pages 4686-4696\"},\"PeriodicalIF\":5.4000,\"publicationDate\":\"2024-08-12\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11323010/pdf/\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Biomacromolecules\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/org/science/article/pii/S1525779724004124\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"BIOCHEMISTRY & MOLECULAR BIOLOGY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Biomacromolecules","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/org/science/article/pii/S1525779724004124","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"BIOCHEMISTRY & MOLECULAR BIOLOGY","Score":null,"Total":0}
Molecularly Engineered Supramolecular Thermoresponsive Hydrogels with Tunable Mechanical and Dynamic Properties
Synthetic supramolecular polymers and hydrogels in water are emerging as promising biomaterials due to their modularity and intrinsic dynamics. Here, we introduce temperature sensitivity into the nonfunctionalized benzene-1,3,5-tricarboxamide (BTA-EG
4
) supramolecular system by incorporating a poly(N-isopropylacrylamide)-functionalized (BTA-PNIPAM) moiety, enabling 3D cell encapsulation applications. The viscous and structural properties in the solution state as well as the mechanical and dynamic features in the gel state of BTA-PNIPAM/BTA-EG
4
mixtures were investigated and modulated. In the dilute state (c ∼μM), BTA-PNIPAM acted as a chain capper below the cloud point temperature (Tcp = 24 °C) but served as a cross-linker above Tcp. At higher concentrations (c ∼mM), weak or stiff hydrogels were obtained, depending on the BTA-PNIPAM/BTA-EG 4
ratio. The mixture with the highest BTA-PNIPAM ratio was ∼100 times stiffer and ∼10 times less dynamic than BTA-EG
4
hydrogel. Facile cell encapsulation in 3D was realized by leveraging the temperature-sensitive sol–gel transition, opening opportunities for utilizing this hydrogel as an extracellular matrix mimic.
期刊介绍：
Biomacromolecules is a leading forum for the dissemination of cutting-edge research at the interface of polymer science and biology. Submissions to Biomacromolecules should contain strong elements of innovation in terms of macromolecular design, synthesis and characterization, or in the application of polymer materials to biology and medicine.
Topics covered by Biomacromolecules include, but are not exclusively limited to: sustainable polymers, polymers based on natural and renewable resources, degradable polymers, polymer conjugates, polymeric drugs, polymers in biocatalysis, biomacromolecular assembly, biomimetic polymers, polymer-biomineral hybrids, biomimetic-polymer processing, polymer recycling, bioactive polymer surfaces, original polymer design for biomedical applications such as immunotherapy, drug delivery, gene delivery, antimicrobial applications, diagnostic imaging and biosensing, polymers in tissue engineering and regenerative medicine, polymeric scaffolds and hydrogels for cell culture and delivery.
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