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Thermoresponsive tetrablock terpolymers: effect of architecture and composition on Gelling behavior

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Constantinou Thermoresponsive Tetrablocks Supporting Information August 2018 revised.pdfSupporting information419.73 kBAdobe PDFView/Open
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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