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Thermoresponsive tetrablock terpolymers: effect of architecture and composition on Gelling behavior
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Title: | Thermoresponsive tetrablock terpolymers: effect of architecture and composition on Gelling behavior |
Authors: | Constantinou, A Sam-Soon, N Carroll, D Georgiou, T |
Item Type: | Journal Article |
Abstract: | Thermoresponsive gels are an exciting class of materials with many bioapplications, like tissue engineering and drug delivery, but they are also used in formulation industry and 3-D printing. For these applications to be feasible, the gelation temperature must be tailored. Here, it is reported how the gelation temperature is affected and can be tailored by varying the architecture of tetrablock terpolymers. Specifically, 15 copolymers based on penta(ethylene glycol) methyl ether methacrylate (PEGMA, A block), n-butyl methacrylate (BuMA, B block), and the thermoresponsive 2-(dimethylamino)ethyl methacrylate (DMAEMA, C block) were synthesized using group transfer polymerization. Nine tetrablock copolymers of varying architectures, and one triblock copolymer for comparison, with constant molar mass and composition were fabricated. Specifically, the polymers that were investigated are (i) three polymers that contain two A blocks (ABCA, ABAC, and ACAB), (ii) three polymers that contain two B blocks (BACB, BABC, and ABCB), (iii) three polymers that contain two C blocks (CABC, CACB, and ACBC), and (iv) one ABC triblock terpolymer that was synthesized as the control polymer. Then, the five more promising architectures were chosen, and five more polymers with a slightly different composition were synthesized and characterized. Interestingly, it was demonstrated that the block position (architecture) has a significant effect on self-assembly (micelle formation), cloud point, and the rheological and gelling properties of the polymers with two of the tetrablocks showing promise as injectable gels. Specifically, the ACBC terpolymer with 20–30–50 w/w % PEGMA–BuMA–DMAEMA formed gels at at lower concentration but at higher temperatures than the ABC triblock copolymer that was synthesized as a control. On the other hand, the BABC terpolymer with 30–35–45 w/w % PEGMA–BuMA–DMAEMA formed gels at the same concentrations as the ABC triblock control polymer but at lower and more desirable temperatures, slightly below body temperature. |
Issue Date: | 25-Sep-2018 |
Date of Acceptance: | 20-Aug-2018 |
URI: | http://hdl.handle.net/10044/1/63744 |
DOI: | 10.1021/acs.macromol.8b01251 |
ISSN: | 0024-9297 |
Publisher: | American Chemical Society |
Start Page: | 7019 |
End Page: | 7031 |
Journal / Book Title: | Macromolecules |
Volume: | 51 |
Issue: | 18 |
Copyright Statement: | © 2018 American Chemical Society. This is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes. |
Keywords: | Science & Technology Physical Sciences Polymer Science AQUEOUS-SOLUTION CHARACTERIZATION GROUP-TRANSFER POLYMERIZATION AMPHIPHILIC MODEL CONETWORKS ABC TRIBLOCK TERPOLYMERS BIOMEDICAL APPLICATIONS TRANSFECTION REAGENTS STAR ARCHITECTURE BLOCK-COPOLYMERS METHACRYLIC-ACID MOLECULAR-WEIGHT Polymers 03 Chemical Sciences 09 Engineering |
Publication Status: | Published |
Online Publication Date: | 2018-08-31 |
Appears in Collections: | Materials Faculty of Engineering |