Polymer Architecture Effects on Poly(N,N-Diethyl Acrylamide)-b-Poly(Ethylene Glycol)-b-Poly(N,N-Diethyl Acrylamide) Thermoreversible Gels and Their Evaluation as a Healthcare Material. 2022

Peter J Haddow, and Marcelo A da Silva, and Daulet B Kaldybekov, and Cecile A Dreiss, and Ewelina Hoffman, and Victoria Hutter, and Vitaliy V Khutoryanskiy, and Stewart B Kirton, and Najet Mahmoudi, and William J McAuley, and Michael T Cook
Research Centre in Topical Drug Delivery and Toxicology, School of Life and Medical Sciences, University of Hertfordshire, Hatfield, Hertfordshire, AL10 9AB, UK.

Thermoreversible gels which transition between liquid-like and solid-like states when warmed have enabled significant novel healthcare technologies. Poly(N,N-diethyl acrylamide) (PDEA) is a thermoresponsive polymer which can be used as a trigger to form thermoreversible gels, however its use in these materials is limited and crucial design principles are unknown. Herein ABA copolymers with the structure PDEA-b-poly(ethylene glycol) (PEG)-b-PDEA are synthesized to give four block copolymers with varied molecular weight of PDEA and PEG blocks. Rheometry on solutions of the block copolymers reveals that high molecular weight PEG blocks are required to form thermoreversible gels with predominantly solid-like behavior. Furthermore, small-angle X-ray scattering elucidates clear differences in the nanostructure of the copolymer library which can be linked to distinct rheological behaviors. A thermoreversible gel formulation based on PDEA (20 kDa)-b-PEG (10 kDa)-b-PDEA (20 kDa) is designed by optimizing the polymer concentration and ionic strength. It is found that the gel is mucoadhesive, stable, and non-toxic, as well as giving controlled release of a hydrophobic drug. Overall, this study provides insight into the effect of polymer architecture on the nanostructure and rheology of PDEA-b-PEG-b-PDEA and presents the development of a highly functional thermoreversible gel with high promise for healthcare applications.

UI MeSH Term Description Entries
D011092 Polyethylene Glycols Polymers of ETHYLENE OXIDE and water, and their ethers. They vary in consistency from liquid to solid depending on the molecular weight indicated by a number following the name. They are used as SURFACTANTS, dispersing agents, solvents, ointment and suppository bases, vehicles, and tablet excipients. Some specific groups are NONOXYNOLS, OCTOXYNOLS, and POLOXAMERS. Macrogols,Polyoxyethylenes,Carbowax,Macrogol,Polyethylene Glycol,Polyethylene Oxide,Polyethyleneoxide,Polyglycol,Glycol, Polyethylene,Glycols, Polyethylene,Oxide, Polyethylene,Oxides, Polyethylene,Polyethylene Oxides,Polyethyleneoxides,Polyglycols,Polyoxyethylene
D011108 Polymers Compounds formed by the joining of smaller, usually repeating, units linked by covalent bonds. These compounds often form large macromolecules (e.g., BIOPOLYMERS; PLASTICS). Polymer
D003695 Delivery of Health Care The concept concerned with all aspects of providing and distributing health services to a patient population. Delivery of Dental Care,Health Care,Health Care Delivery,Health Care Systems,Community-Based Distribution,Contraceptive Distribution,Delivery of Healthcare,Dental Care Delivery,Distribution, Non-Clinical,Distribution, Nonclinical,Distributional Activities,Healthcare,Healthcare Delivery,Healthcare Systems,Non-Clinical Distribution,Nonclinical Distribution,Activities, Distributional,Activity, Distributional,Care, Health,Community Based Distribution,Community-Based Distributions,Contraceptive Distributions,Deliveries, Healthcare,Delivery, Dental Care,Delivery, Health Care,Delivery, Healthcare,Distribution, Community-Based,Distribution, Contraceptive,Distribution, Non Clinical,Distributional Activity,Distributions, Community-Based,Distributions, Contraceptive,Distributions, Non-Clinical,Distributions, Nonclinical,Health Care System,Healthcare Deliveries,Healthcare System,Non Clinical Distribution,Non-Clinical Distributions,Nonclinical Distributions,System, Health Care,System, Healthcare,Systems, Health Care,Systems, Healthcare
D005782 Gels Colloids with a solid continuous phase and liquid as the dispersed phase; gels may be unstable when, due to temperature or other cause, the solid phase liquefies; the resulting colloid is called a sol.
D013696 Temperature The property of objects that determines the direction of heat flow when they are placed in direct thermal contact. The temperature is the energy of microscopic motions (vibrational and translational) of the particles of atoms. Temperatures
D020100 Hydrogels Water swollen, rigid, 3-dimensional network of cross-linked, hydrophilic macromolecules, 20-95% water. They are used in paints, printing inks, foodstuffs, pharmaceuticals, and cosmetics. (Grant & Hackh's Chemical Dictionary, 5th ed) Hydrogel,In Situ Hydrogel,In Situ Hydrogels,Patterned Hydrogel,Patterned Hydrogels,Hydrogel, In Situ,Hydrogel, Patterned
D020106 Acrylamide A colorless, odorless, highly water soluble vinyl monomer formed from the hydration of acrylonitrile. It is primarily used in research laboratories for electrophoresis, chromatography, and electron microscopy and in the sewage and wastewater treatment industries.

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