Investigation of the thermogelation of a promising biocompatible ABC triblock terpolymer and its comparison with pluronic F127
File(s) ma-2021-02123f.R2_Proof_hi accepted version.pdf (2.93 MB) Constantinou OBD vs F127 SANS ESI Jan 2022 .pdf (1.68 MB)
Accepted version
Supporting information
Author(s)
Type
Journal Article
Abstract
Thermoresponsive polymers with the appropriate structure form physical networks upon changes in temperature, and they find utility in formulation science, tissue engineering, and drug delivery. Here, we report a cost-effective biocompatible alternative, namely OEGMA30015-b-BuMA26-b-DEGMA13, which forms gels at low concentrations (as low as 2% w/w); OEGMA300, BuMA, and DEGMA stand for oligo(ethylene glycol) methyl ether methacrylate (MM = 300 g mol–1), n-butyl methacrylate, and di(ethylene glycol) methyl ether methacrylate, respectively. This polymer is investigated in depth and is compared to its commercially available counterpart, Poloxamer P407 (Pluronic F127). To elucidate the differences in their macroscale gelling behavior, we investigate their nanoscale self-assembly by means of small-angle neutron scattering and simultaneously recording their rheological properties. Two different gelation mechanisms are revealed. The triblock copolymer inherently forms elongated micelles, whose length increases by temperature to form worm-like micelles, thus promoting gelation. In contrast, Pluronic F127’s micellization is temperature-driven, and its gelation is attributed to the close packing of the micelles. The gel structure is analyzed through cryogenic scanning and transmission electron microscopy. Ex vivo gelation study upon intracameral injections demonstrates excellent potential for its application to improve drug residence in the eye.
Date Issued
2022-02-14
Date Acceptance
2022-01-28
Citation
Macromolecules, 2022, 55 (5), pp.1783-1799
ISSN
0024-9297
Publisher
American Chemical Society (ACS)
Start Page
1783
End Page
1799
Journal / Book Title
Macromolecules
Volume
55
Issue
5
Copyright Statement
© 2022 American Chemical Society. . This document is the Accepted Manuscript version of a Published Work that appeared in final form in Macromolecules, after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acs.macromol.1c02123
Sponsor
Engineering & Physical Science Research Council (E
Engineering & Physical Science Research Council (E
ISIS Neutron & Muon Source
Engineering and Physical Sciences Research Council
Ovarian Cancer Action
Identifier
https://pubs.acs.org/doi/10.1021/acs.macromol.1c02123
Grant Number
EP/R511547/1
MMRE_P75852
REF2021
EP/R511547/1
n/a
Subjects
Science & Technology
Physical Sciences
Polymer Science
GROUP-TRANSFER POLYMERIZATION
2-(2-METHOXYETHOXY)ETHYL METHACRYLATE
THERMORESPONSIVE HYDROGELS
TRANSFECTION EFFICIENCY
NEUTRON-SCATTERING
PHASE-TRANSITIONS
AQUEOUS-SOLUTIONS
BLOCK-COPOLYMERS
HIGHLY EFFICIENT
MOLECULAR-WEIGHT
Polymers
03 Chemical Sciences
09 Engineering
Publication Status
Published
Article Number
acs.macromol.1c02123
Date Publish Online
2022-02-14
