Thermoresponsive Multiblock Copolymers: Chemistry, Properties and Applications

Constantinou, Anna P.; Georgiou, Theoni K.

doi:10.1002/9781119157830.ch2

Cited by 6 publications

(6 citation statements)

References 121 publications

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“…Materials that respond to an external stimulus by changing a physical property are named “smart” materials, and they have many fascinating applications in biomedical science, − catalysis, − robotics, molecular transport, − as sensors and actuators, − and tools in chromatographic separation. − A special type of smart materials are thermoresponsive materials, which change properties as a result of temperature variations. ,− Thus, in polymer science, the synthesis and characterization of novel thermoresponsive polymers, the properties of which can be tuned by modifications in the polymer structure, are of major focus.…”

Section: Introductionmentioning

confidence: 99%

Tuning the Gelation of Thermoresponsive Gels Based on Triblock Terpolymers

2021

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In need of new thermoresponsive gels, a novel combination of repeated units is reported in this study, with the best-performing polymer outperforming the commercial counterpart pluronic F127 by gelling at body temperatures at concentrations as low as 3 w/w%. These polymers are ABC triblock terpolymers of constant molar mass (MM), where A, B, and C blocks consist of hydrophilic oligo(ethylene glycol) methyl ether methacrylate with an average molar mass of 300 g mol–1 (OEGMA300), hydrophobic n-butyl methacrylate (BuMA), and the thermoresponsive di(ethylene glycol) methyl ether methacrylate (DEGMA), respectively. In total, 15 triblock terpolymers were synthesized via group transfer polymerization (GTP), and their composition was systematically varied. Key focus was the characterization of their gelation properties via visual tests and rheological measurements. It was concluded that achieving the optimum hydrophilicity/hydrophobicity ratio is critical to ensure a clear solution to gel transition and a wide gelation area that includes the body temperature.

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Section: Introductionmentioning

confidence: 99%

Tuning the Gelation of Thermoresponsive Gels Based on Triblock Terpolymers

2021

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“…Thermoresponsive polymers are widely studied by scientists around the world, as they do present interesting changes in their properties depending on the temperature. [1][2][3][4][5] Thermoresponsive polymers can either be chemically crosslinked, thus forming thermoresponsive polymeric networks (also known as chemically crosslinked gels), or can be studied without further chemical crosslinking. [3] In both cases, they are categorised in two groups, depending on how their compatibility with the solvent varies with the temperature.…”

Section: Introductionmentioning

confidence: 99%

Tricomponent thermoresponsive polymers based on an amine-containing monomer with tuneable hydrophobicity: Effect of composition

Constantinou

Lan

Carroll

et al. 2020

European Polymer Journal

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In the present study, six dual-responsive ABC triblock copolymers were synthesised via group transfer polymerisation (GTP) and investigated through visual inspections in terms of their thermoresponsive behaviour. The copolymers consist of i) penta(ethylene glycol) methyl ether methacrylate (PEGMA), which is hydrophilic and thermoresponsive at high temperatures, ii) n-butyl methacrylate (BuMA) as the hydrophobic counterpart to promote self-assembly, and iii) 2-(diethylamino)ethyl methacrylate (DEAEMA), which is pH-responsive by adjusting its hydrophilicity depending on the pH. The effect of the degree of ionisation of DEAEMA units as well as the ionic strength effect on the self-assembly behaviour of the copolymers was tested via dynamic light scattering (DLS). The dissociation constants (pKa) of the amine units of DEAEMA were determined via potentiometric titrations. The thermoresponse has been primarily been investigated in means of cloud points (CPs) at various pH values in deionised water. Detailed phase diagrams were constructed for all the polymer solutions in phosphate buffered saline (PBS), with the interest being focused on the gelation area. It has been clearly proven that gelation is promoted as the content in BuMA and DEAEMA is increased. The polymer that presented the widest gelation area has been further investigated via rheology in terms of its gelation temperature, gelation time and shear-thinning properties.

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“…Stimulus-responsive polymers are polymers that respond to an external stimulus [1,2]. When this stimulus is temperature, the polymers are called thermoresponsive or temperatureresponsive [3][4][5][6][7]. In some cases, when the temperature is varied, a polymer network is formed, which is called thermoresponsive gel.…”

Section: Introductionmentioning

confidence: 99%

Homopolymer and ABC Triblock Copolymer Mixtures for Thermoresponsive Gel Formulations

Constantinou

Provatakis

et al. 2021

Gels

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Our group has recently invented a novel series of thermoresponsive ABC triblock terpolymers based on oligo(ethylene glycol) methyl ether methacrylate with average Mn 300 g mol‒1 (OEGMA300, A unit), n-butyl methacrylate (BuMA, B unit) and di(ethylene glycol) methyl ether methacrylate (DEGMA, C unit) with excellent thermogelling properties. In this study, we investigate how the addition of OEGMA300x homopolymers of varying molar mass (MM) affects the gelation characteristics of the best performing ABC triblock terpolymer. Interestingly, the gelation is not disrupted by the addition of the homopolymers, with the gelation temperature (Tgel) remaining stable at around 30 °C, depending on the MM and content in OEGMA300x homopolymer. Moreover, stronger gels are formed when higher MM OEGMA300x homopolymers are added, presumably due to the homopolymer chains acting as bridges between the micelles formed by the triblock terpolymer, thus, favouring gelation. In summary, novel formulations based on mixtures of triblock copolymer and homopolymers are presented, which can provide a cost-effective alternative for use in biomedical applications, compared to the use of the triblock copolymer only.

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Thermoresponsive Multiblock Copolymers: Chemistry, Properties and Applications

Cited by 6 publications

References 121 publications

Tuning the Gelation of Thermoresponsive Gels Based on Triblock Terpolymers

Tuning the Gelation of Thermoresponsive Gels Based on Triblock Terpolymers

Tricomponent thermoresponsive polymers based on an amine-containing monomer with tuneable hydrophobicity: Effect of composition

Homopolymer and ABC Triblock Copolymer Mixtures for Thermoresponsive Gel Formulations

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